Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 23
·10856-10867
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IF 9.931
Xiangzhong Ren,Moujie Huang,Shan Luo,Yongliang Li,Libo Deng,Hongwei Mi,Lingna Sun,Peixin Zhang
A novel free-standing and binder-free air electrode with excellent electrochemical performance was designed for highly reversible Li–O2 batteries. The 3D hierarchically N, S co-doped macro–mesoporous carbon (NSMmC) was deposited on carbon paper (CP) via a template method, and then uniformly decorated with PdNi nanoparticles. The macropores of the porous carbon can provide enough space to accommodate discharge products, while the interconnected pores and channels efficiently facilitate oxygen and electrolyte diffusion. The introduction of PdNi nanoparticles greatly reduce the charge transfer resistance, resulting in the improvement of electron mobility of the whole cathode. Compared with Pd–NSMmC/CP and NSMmC/CP cathodes, the PdNi–NSMmC/CP cathode shows considerable enhancement of Li–O2 battery performance. The ultrafine and evenly distributed PdNi nanoparticles can not only provide enough catalytic sites, but can also tailor the discharge products into a cage-like morphology, which provides enough channels for electron and lithium ion transport. Moreover, the smaller size of the cage-like Li2O2 makes it decompose more easily, resulting in lower charge overpotential. This study provides a promising strategy to design 3D structured air cathodes for Li–O2 batteries with high electrocatalytic performance.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Yufeng Da,Yong Liu,Yong Chen,Rui Han,Jianlong Wang
Recently, the activation of molecular oxygen (O 2 ) by graphite (Gr) supported aluminum (Al) composite for the in-situ generation of H 2 O 2 / OH gains increasing attention. However, the limited O 2 mass transfer and low catalytic activity of decomposition H 2 O 2 at neutral pH restrict its further application in the wastewater treatment. In this work, a novel N-rich graphite supported aluminum (Al-Gr-NPC) composite was fabricated by introducing the nitrogen-rich porous carbon (NPC) obtained from ZIF-8 derivative as precursor, and by a ball-milling and sintering process. The results showed that the NPC introduction not only improved the physiochemical property of Al-Gr, such as specific surface area, pore structure and hydrophobicity, facilitating the mass transfer of O 2 , but also made Al-Gr contain plentiful N species, serving as active sites for the two-electron ORR process and catalytic decomposition of H 2 O 2 . These excellent performances of Al-Gr-NPC favored the production and utilization of H 2 O 2 by the activation of O 2 at neutral pH and air aeration. The carbonization temperature of ZIF-8 determined the type of N species, surface area and the hydrophobicity of NPC. 1 O 2 was the main oxidant for tetracycline hydrochloride (TC) degradation. 100 % TC degradation and 60.57 % of TOC removal were achieved within 60 min at neutral pH, Al-Gr-NPC dosage of 0.5 g/L and initial TC concentration of 20 mg/L. The toxicity of the final products of TC degradation were much lower than TC by ECOSAR software analysis. Al-Gr-NPC could be used for the removal of antibiotic contaminants from wastewater.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
·
IF 14.224
Tong Liu,Yang Liu,Peng Zhou,Zhaokun Xiong,Heng Zhang,Chuanshu He,Ye Du,Gang Yao,Bo Lai
As one of the most promising advanced oxidation processes , the activation of S(IV) by iron-based materials to produce SO 4 •− has become a hot technology for the degradation of organic pollutants . However, the mechanism of radical chain reactions has not been clearly explored. Herein, we established a novel AOP system based on the combination of zero-valent iron (ZVI) and potassium pyrosulfite (PPS). Combined with the degradation trends of CBZ and the change of DO concentration, the system was proposed to be divided into a slow initiation stage in 5 min and a rapid degradation stage in 5 − 10 min. Through a series of quenching experiments, electron paramagnetic resonance tests and several probe experiments, the mechanisms of two radical chain reactions were proposed between ZVI and PPS: the first one produced O 2 •− and HO • , and the other produced SO 3 •− , SO 5 •− , SO 4 •− and HO • . The two-stage reaction and two radical production paths of the ZVI/PPS system were proposed for the first time, which provided theoretical guidance for the practical application of the ZVI/PPS system. The ZVI/PPS system has been found to have excellent environmental adaptability in the treatment of industrial wastewater .
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Gangning Zhang,Shigang Lu,Shangqian Zhao,Li Zhang,Haobo Sun
Due to the theoretical ultrahigh energy density of the Li–O2 battery chemistry, it has been hailed as the ultimate battery technology. Yet, practical Li–O2 batteries usually need to be designed in a large-sized pattern to actualize a high specific energy density, and such batteries often cannot be cycled effectively. To understand the inherent reasons, we specially prepared large-sized (13 cm × 13 cm) Li–O2 model batteries with practical energy output (6.9 Ah and 667.4 Wh/kgcell) for investigations. By subregional and postmortem analysis, the cathode interface was found to have severe local inhomogeneity after discharge, which was highly associated with the electrolyte and O2 maldistribution. The quantitative results by X-ray photoelectron spectroscopy (XPS) evidenced that this local inhomogeneity can exacerbate the generation of lithium acetate during charge, where the locally higher ratio of unutilized carbon surface and less Li2O2 after discharge would result in increased lithium acetate formation for a subsequent local overcharge. Moreover, verification experiments proved that the byproduct lithium acetate, which had been of less concern, was recalcitrant and triggered much larger polarization compared with the commonly reported byproduct Li2CO3 during battery operations, further revealing the key limiting factors leading to the poor rechargeability of batteries by its accumulation at a pouch-type cell level.
研究领域:
材料科学
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电化学
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JOURNAL OF POWER SOURCES
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2019
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IF 7.467
Jia Liu,Tong Wu,Siqi Zhang,Dan Li,Ying Wang,Haiming Xie,Jinghai Yang,Guiru Sun
One big obstacle for a redox mediator (RM)-based Li–O 2 system is the redox shuttling between the diffusible RM + and Li anode, leading to the unexpected RM degradation and continuous deterioration of Li anode, which inevitably results in a low energy efficiency and a poor cycling stability for the Li–O 2 battery. Here, InBr 3 as a self-defensed RM is firstly introduced into Li–O 2 batteries, which can lower the cell overpotential and thus improve the cycling performance. Moreover, due to the In 3+ existence, an In-rich composite protective layer can be in situ generated on the Li anode, which contributes to suppressing the redox shuttling, improving the interface stability of Li and electrolyte, and inhibiting the dendrite formation. This work gives an insight into the development of self-defensed RM and the protection of the Li anode for Li–O 2 batteries.
研究领域:
储能
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电化学
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材料科学
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电池技术
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Catalysts
·
2026
·Vol. 16
·期 5
·417
·
IF 4.5
Ziyan Mi,Huayun Long,Yuhua Jia,Yue Ma,Cuilan Miao,Yan Xie,Xiaomei Zhu,Jiahui Huang
Developing effective catalysts for the epoxidation of propylene with H2and O2holds significant scientific and industrial significance. This study synthesized a series of Au/TS-1 catalysts modified with alkali metals (Na+, Cs+) and carefully examined their impact on gas-phase propylene epoxidation, with particular attention to the role of anions. The optimal Au–CsC(1:10)/TS-1 catalyst (Cs2CO3modified, Au/Cs molar ratio = 1:10) achieves a propylene conversion of 16.8%, a PO selectivity of 88.5%, an H2efficiency of 40.8%, a record PO formation rate of 383.9 gpo·kgcat−1·h−1, and unprecedented long term stability (>380 h without deactivation). To the best of our knowledge, no previous study has simultaneously achieved such balanced and outstanding performance across all these key indicators. Comprehensive characterization reveals that Cs+modification suppresses side reactions and coke formation, increases microporosity, tunes surface acid–base properties and hydrophobicity, restricts Au particle size, and stabilizes both Au0and tetra coordinated Ti sites, thereby inhibiting H2O2decomposition and PO isomerization while greatly enhancing reaction efficiency. This holistic advancement represents a significant leap forward for Au based catalysts in gas phase propylene epoxidation, offering both a theoretical foundation and practical guidance for the development of high performance epoxidation catalysts.
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ANALYTICAL CHEMISTRY
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2026
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IF 7.3
Yuhan Chen,Boyan Wang,Yafei Du,Yaru Zhang,Ying Zhang,Lu Bai,Serge Cosnier,Bo Liang,Aihua Liu
Enzymatic biofuel cell (EBFC) is an electrochemical device that uses enzymes to convert the chemical energy of renewable biomass into electrical energy. However, improving the EBFC performance, such as the cost-effectiveness, operational stability, output power density (Pmax), and open circuit voltage (OCV), remains challenging. Especially, the activity and stability of enzymes, substrate tolerance, cost, and immobilization strategy are crucial in developing EBFCs. Herein, we report on MnO2 nanosheets (MnO2 NSs) prepared via facile chemical precipitation, exhibiting outstanding laccase-mimicking activity with good stability and excellent resistance to halide ions. Then, for the first time, the laccase-like nanozyme could replace natural laccase as a cathode catalyst for efficient oxygen reduction reaction under nearly neutral pH condition, which exhibits an onset potential of 841 mV vs NHE in O2 reduction mediated by 2,2-bisazo-bis(3-ethyl-benzothiazole-6-sulfonic acid) diammonium salt. In addition, cascade enzymes of polyphosphate glucokinase (PPGK) and glucose 6-phosphate dehydrogenase (G6PDH) were successfully displayed on the Escherichia coli (E. coli) surface. The resultant PPGK-E. coli can catalyze the oxidation of glucose to glucose-6-phosphate (G6P), which can be subsequently oxidized by G6PDH-E. coli in the presence of the coenzyme NAD+ efficiently and converted to NADH. Finally, a dual-chamber glucose/O2 EBFC was constructed with PPGK-E. coli/G6PDH-E. coli (2:1) as the anodic catalyst and an MnO2 NS-based cathodic catalyst. The bacterial surface-displayed enzymes were kept in an anodic solution, which could not only retain the enzyme activity but also ensure mass transfer efficiency, thereby greatly enhancing the enzyme's inherent catalytic potential. The as-developed EBFC achieved an OCV of 0.68 V and a Pmax of 32.2 μW/cm2 as well as good operational stability. The strategies proposed provide new ideas for constructing high-performance EBFCs using other nanozymes and biocatalysts, which may provide new avenues for the development and utilization of sustainable energy for promising applications in wearable devices or in self-powered sensors.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Haoran Yu,Changmin Liu,Shuo Liu,Yu Gu,Shuya Wang,Ali Yaraş,Linchao Hu,Wenyi Zhang,Mingguo Peng,Hasan Arslanoğlu,Linqiang Mao
Spent petroleum refining catalyst is regarded as the important secondary resource for valuable metals. However, common recycling strategies, including soda roasting, acid and alkaline solutions leaching and chemically precipitation, produced large quantities of high salinity wastewater. This study proposed an efficient method to recovery of Mo and Ni from the spent hydrodesulfurization (HDS) catalyst via O 2 -rich roasting and organic acid leaching with the advantage of less salinity wastewater production. The transformation of Mo(IV) into soluble Mo(VI) was enhanced by O 2 -rich atmosphere roasting, and 98.64% of Mo(IV) was oxidized at 650 ℃ for 2 h in atmosphere containing 30% of O 2 . The oxidation process of Mo(IV) was agreed with the shrinkage pore model, and regulated by surface reaction and internal diffusion. 97.97% of Mo(VI) was leached from roasted product by oxalic acid , separated with complexation extraction agent of Ala-TBP and recovered as (NH 4 ) 8 Mo 10 O 34 and (NH 4 ) 2 Mo 3 O 10 by evaporative crystallization. Ni was leached out from spent catalyst with 1 mol/L acetic acid, and precipitated as NiC 2 O 4 with oxalic acid . 95.92% of Mo and 96.77% of Ni were recovered from spent HDS catalyst with this recycling route. This study provided a high-efficient and eco-friendly method to recovery of valuable metals from spent catalyst.
研究领域:
环境科学
·
冶金工程
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Small
·
2024
·
IF 13
Nan Wang,Tingxue Fang,Tinghui An,Yuhao Wang,Jiaqi Li,Shuming Yu,Honghai Sun,Dong Xiang,Xiangjie Bo,Kedi Cai
Li-O 2 batteries urgently needs high discharge capacity and stable cycling performance, requiring effective and reliable bifunctional catalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Herein, Hovenia acerba Lindl -like heterostructure composed of cobalt sulfide and tin dioxide supported on carbon substrate (CoS/SnO 2 @C) is prepared via CO 2 laser irradiation technology. The half-wave potential of CoS/SnO 2 @C for the ORR is 0.88 V, while the overpotential of the OER at 10 mA cm −2 is as low as 270 mV. The Li-O 2 batteries employing the bifunctional CoS/SnO 2 @C catalyst displays a high discharge specific capacity of 3332.25 mAh g −1 and long cycling life of 226 cycles. Additionally, theory calculations demonstrate that the construction of heterostructure decreases energy barrier of the rate-determining step (RDS) for both ORR and OER. Notably, SnO 2 behaves as the electronic promoter to optimize the electronic structure of heterostructure interface and triggers charge redistribution of CoS, which weakens the adsorption strength of the * O-intermediates and allows to break the linear scaling relationship, thus further enhancing the catalytic performance of CoS/SnO 2 @C. This research furnishes directions for the design of heterogeneous catalysts, highlighting its great potential for application in rechargeable Li-O 2 batteries.
研究领域:
材料科学
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电化学
·
能源存储与转换
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高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-19
·
IF 15.7
Tang Yizhang,Yu Xujiang,He Liangrui,Tang Meng,Yue Wenji,Chen Ruitong,Zhao Jie,Pan Qi,Li Wanwan
Reactive oxygen species with evoked immunotherapy holds tremendous promise for cancer treatment but has limitations due to its dependence on exogenous excitation and/or endogenous H 2 O 2 and O 2 . Here we report a versatile oxidizing pentavalent bismuth(V) nanoplatform (NaBi V O 3 -PEG) can generate reactive oxygen species in an excitation-free and H 2 O 2 - and O 2 -independent manner. Upon exposure to the tumor microenvironment, NaBi V O 3 -PEG undergoes continuous H + -accelerated hydrolysis with •OH and 1 O 2 generation through electron transfer-mediated Bi V -to-Bi III conversion and lattice oxygen transformation. The simultaneous release of sodium counterions after endocytosis triggers caspase-1-mediated pyroptosis. NaBi V O 3 -PEG intratumorally administered initiates robust therapeutic efficacies against both primary and distant tumors and activates systemic immune responses to combat tumor metastasis. NaBi V O 3 -PEG intravenously administered can efficiently accumulate at the tumor site for further real-time computed tomography monitoring, immunotherapy, or alternative synergistic immune-radiotherapy. Overall, this work offers a nanomedicine based on high-valence bismuth(V) nanoplatform and underscores its great potential for cancer immunotherapy.
研究领域:
纳米医学
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癌症免疫疗法
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肿瘤学
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材料科学
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生物医学工程
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
·
IF 8.6
Fan Liu,Jing Ding,Qingliang Zhao,Guanshu Zhao,Kun Wang,Lili Li,Shuyan Guan
Advance oxidation process (AOP) is a promising way for micropollutants treatment, but the consumption of chemicals and energies limits its large-scale application. To address this issue, a novel boron-doped biochar (BBC) system was developed for the efficient removal of micropollutants, requiring no external energy or oxidant. Herein we demonstrated that the synthesized BBC could efficiently activate the dissolved oxygen (O 2 ) in the water or oxidize micropollutant directly. The complete sulfamethoxazole (SMX) could be removed within 30 min by the BBC synthesized at 600 °C (BBC-600). The experiments on material characterization and removal performance with quenchers revealed that the introduction of boron into biochar increased the active sites for O 2 activation, including persistent free radicals (PFRs) and boron moieties (BC 3 , BCO 2 , and BC 2 O) on the biochar. The generated reactive oxidation species (ROS), mainly O 2 − , were responsible for the SMX degradation in this BBC system. Different performance of aged experiments in air and N 2 conditions indicated that PFRs could also directly oxidize SMX. Density functional theory (DFT) was used to further illustrate the inner mechanism of enhanced electron transfer via boron moieties for O 2 activation and SMX degradation. Electrons of the adsorbed micropollutant could be transferred to boron moieties, and then trapped by O 2 in water to produce O 2 − and 1 O 2 for SMX degradation. This study provided a new insight into the structure–activity relationship of B-doped biochar for the direct and indirect degradation of micropollutant, and opened a new avenue for micropollutant degradation without external energy and oxidant.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 8
·3936-3944
·
IF 3.3
Binxiong Guang,Yiwei Zhang,Yahui Xiao,Miaojun Su,Yong Liu
To bridge transition metal complexes and heterogeneous catalysts for allylic oxidation of cyclohexene to 2-cyclohexene-1-one with O2 under mild conditions, Cu(II) coordinated N-bearing heteropolyacid-based poly(ionic liquid)s (Cu-PDVD-PW) were herein synthesized as novel heterogeneous catalysts. The physicochemical properties of the catalysts were investigated by BET, TG, XPS, FT-IR and SEM/EDS analysis. The results indicated that the as-prepared Cu-PDVD-PW catalyst inherited appreciable mesopores and excellent thermal stability from the N-bearing poly(ionic liquid)s, which could increase the mass transfer rate and provide more accessible active sites. Significantly, the Cu2+ cations were homogeneously and stably coordinated on the N-bearing poly(ionic liquid)s, which greatly improved the catalytic performance for cyclohexene oxidation toward 2-cyclohexene-1-one with O2 under mild conditions. Specifically, the 3% Cu-PDVD-PW catalyst exhibited 75.9% conversion of cyclohexene with a selectivity towards 2-cyclohexene-1-one of 45.5% and no activity loss within five cycles under the optimum reaction conditions.
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