JOURNAL OF HAZARDOUS MATERIALS
·
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 .
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
VACUUM
·
2023
·
IF 4
Chaoqun Yan,Zhiliang Cheng,Xuan Zhang,Juan Wei,Qian Xu
The photocatalytic efficiency of hematite (α-Fe 2 O 3 ) is limited by its photoexcited state lifetime and diffusion length. By adjusting the surface structure, the photogenerated electron pairs can migrate to the surface and the charge recombination can be suppressed, which can effectively solve these problems and improve the photo-Fenton performance. In this study, four kinds different morphologies of α-Fe 2 O 3 - x (truncated hexagonal bipyramidal, cubic, hexagonal shape, and spherical) were synthesized by hydrothermal method , and a photocatalyst (H-α-Fe 2 O 3 - x ) with higher catalytic activity was prepared by hydrogenation. The results of UV–Vis DRS , PL , Raman, and XPS analysis , the oxygen vacancies and Fe (II) species were introduced into the α-Fe 2 O 3 catalyst after the hydrogenation reaction. The H-α-Fe 2 O 3 - x showed good degradation performance for TC and DX as EMPs model pollutants. The results show that the formation of oxygen vacancy and Fe 2+ is the main factor to improve the photocatalytic activity of the reaction system. Furthermore, the reaction mechanism revealed that reactive radicals involved in the H-α-Fe 2 O 3 - x photocatalytic system were •OH, •O 2 − , and h + responsible. This study provides an alternative technology for an easy and effective means for bandgap engineering to improve the photocatalytic performance of photocatalysts and facilitate widening environmental application.
研究领域:
环境科学
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材料科学
·
化学
·
光催化
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Yifeng Zhang,Shuo Zhang,Haorong Sun,Zhe Wang,Feixue Gao,Jiawei Zhang,Zezheng Liu,Ming Fang,Xiaoli Tan,Xiangke Wang
Photocatalytic U(VI) extraction is considered as the most promising way to solve the current shortage of uranium resources and radioactive contamination. In this work, O-doped hexagonal-cubic CdS phase heterojunction was constructed by a simple thermal treatment and was successfully used for the photoextraction of U(VI) from water bodies. The samples with different heat treatment temperatures have different phase ratios and oxygen doping amounts. The experimental results show that the CdS heat treated at 350 °C (CdS-350) has the best photocatalytic activity, which can extract 80% of uranium within 120 min (m/v CdS-350 = 0.4 mg/g, C U(VI) = 50 ppm). More interestingly, a systematic mechanistic investigation shows that the extraction process is divided into two steps: i.e., photoelectrons and • O 2 − reducing U(VI) to U(IV) first, followed by photoholes and • OH oxidizing U(IV) to insoluble U(VI) (UO 2 (OH) 2 ). The second step of oxidation allows CdS-350 to avoid photocorrosion, resulting in an excellent recycling performance of only 8% decrease in performance after four cycles.
研究领域:
环境科学
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材料科学
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化学
✓ 已验证
产品关联
DOI
高影响因子
TALANTA
·
2021
·
IF 6.057
Xiaoqi Zhu,Lingli Xuan,Jiawei Gong,Junjie Liu,Xiaobo Wang,Fengna Xi,Jie Chen
Direct, rapid and sensitive detection of physiologically-relevant active small molecules (ASMs) in complex biological samples is highly desirable. Herein, we present an electrochemical sensing platform by combining three-dimensional macroscopic graphene (3DG) and vertically-ordered mesoporous silica-nanochannel film (VMSF), which is able to directly detect ASMs in complex samples with high sensitivity and no need of tedious pretreatment. Free-standing and macroscopic 3DG serves as the supporting electrode and O 2 -plasma treatment is proposed as a simple and green approach to improve its hydrophilicity and electrochemical activity. The plasma-treated 3DG (pl-3DG) is suitable for stable modification of VMSF using electrochemically assisted self-assembly (EASA) method, conferring the electrode (VMSF/pl-3DG) with excellent anti-fouling properties. As the proof-of-concept demonstration, VMSF/pl-3DG sensor exhibits fast and ultrasensitive determination of uric acid (UA) with ultralow limit of detection (LOD, 23 nM) owing to high active surface, unhindered mass transfer, good electrical transfer of 3DG and signal amplification of VMSF nanochannel . Direct determination of UA in biological sample (serum) is also realized without the need of tedious pretreatment.
研究领域:
材料科学
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分析化学
·
生物医学工程
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纳米技术
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Qiansheng Li,Hong Lu,Xiaolei Wang,Zhongqiang Hong,Ze Fu,Xinxin Liu,Jiti Zhou
Low solar energy utilization, instability of Fe ions and Fe(III)/Fe(II) cycle difficulty are three main factors, limiting the photocatalytic activity of the Fe/peroxymonosulfate (PMS) system. Herein, based on the N and Fe co-doped carbon dots (N, Fe-CDs) synthesized by a facile one-pot hydrothermal method, a new Fe(III)/Fe(II) cycle system for PMS activation under visible light irradiation was proposed. The characterization experiments showed that Fe has been successfully doped to the sp 2 graphitic structure and mainly existed as Fe-N and Fe-OH complexes, which played an important role in harvesting visible light, enhancing the stability of Fe ions and acting as active sites to accelerate electron transfer. Under visible light irradiation, the photogenerated electrons of N, Fe-CDs could be directly transferred to Fe (III) for Fe (II) formation via the ligand-to-mental charge transfer process, thus accelerating the Fe(III)/Fe(II) cycle. When N, Fe-CDs were used for activating PMS under visible light irradiation, aminopyrine could be efficiently degraded and mineralized to CO 2 via the cleavage of pyrazole ring, demethylation, hydroxylation, decarbonylation and the cleavage of benzene ring. The produced O 2 − and 1 O 2 played the main roles in the whole photocatalytic reaction. The above results revealed that the novel N, Fe-CDs could effectively activate PMS under visible light irradiation for the degradation of pharmaceuticals in the polluted water.
研究领域:
环境科学
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光催化
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水处理
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2024
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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
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能源存储与转换
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
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2021
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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
✓ 已验证
DOI
PubMed
高影响因子
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.
✓ 已验证
DOI
高影响因子
ANALYTICAL CHEMISTRY
·
2026
·
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.
✓ 已验证
DOI
PubMed
高影响因子
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
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF POWER SOURCES
·
2019
·
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
·
电化学
·
材料科学
·
电池技术
✓ 已验证
DOI
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
·
癌症免疫疗法
·
肿瘤学
·
材料科学
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生物医学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）