JOURNAL OF HAZARDOUS MATERIALS
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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
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冶金工程
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DOI
PubMed
高影响因子
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
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能源存储与转换
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产品关联
DOI
PubMed
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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产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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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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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2023
·Vol. 47
·期 8
·3936-3944
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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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DOI
高影响因子
BIOSENSORS & BIOELECTRONICS
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2013
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IF 5.437
Lin Liu,Feng Zhao,Fengji Ma,Liping Zhang,Suling Yang,Ning Xia
β-Amyloid (Aβ) peptides are believed to be important for the diagnosis and prognosis of Alzheimer's disease (AD) serving as reliable molecular biomarkers. In this work, we reported a simple and sensitive electrochemical strategy for the detection of total Aβ peptides using gold nanoparticles modified with Aβ(1–16)-heme (denoted as Aβ(1–16)-heme-AuNPs). Monoclonal antibody (mAb) specific to the common N-terminus of Aβ was immobilized onto gold electrode for the capture of Aβ(1–16)-heme-AuNPs. The anchored Aβ(1–16)-heme-AuNPs showed strong electrocatalytic O 2 reduction. Pre-incubation of the mAb-covered electrode with native Aβ decreased the amount of Aβ(1–16)-heme-AuNPs immobilized onto the electrode, resulting in the decrease of the reduction current of O 2 to H 2 O 2 . The competitive assay is sensitive and selective to Aβ peptides. The voltammetric responses were found to be proportional to the concentrations of Aβ ranging from 0.02 to 1.50 nM, and a detection limit of 10 pM was achieved. To demonstrate the viability of the method for the analysis of Aβ in real sample, artificial cerebrospinal fluid (aCSF) containing Aβ(1–40), Aβ(1–42) and Aβ(1–16) was tested. We believe that the method would offer a useful means for quantifying Aβ in a biological matrix, and be valuable in the design of new types of electrochemical biosensors for the detection of peptides and proteins.
研究领域:
生物医学
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神经科学
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分析化学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Dan Li,Changyan Zhu,Min Zhang,Ying Wang,Ziye Kang,Yulong Liu,Jun Liu,Jia Liu,Haiming Xie
How to develop a homogeneous redox mediator (RM) towards both ORR and OER and how to prevent the shuttle effect are two main issues for Li-O 2 batteries thus far. Here, we firstly report 1,2-dimethyl-3-propylimidazolium iodide (DMPII), which serves multiple functions as a RM for discharge capacity promotion, a RM for charge potential reduction, and a Li anode protector for shuttling suppression by in situ generating a “self-defensed” SEI layer. Benefiting from these advantages, a cell with DMPII displays a stable cyclability with a low terminal charge potential of ~3.6 V till the cell death, a considerable rate performance, and a good reversibility associated with Li 2 O 2 formation and degradation. Based on the experimental and density functional theory (DFT) calculation results, a working mechanism for a cell operation is also proposed. These results represent a promising progress in the development of multiple-functional RM for Li-O 2 batteries. Moreover, we expect that this work gives an insight into the in situ protection of Li metal anode for board applications ( e.g., Li-S batteries, all-solid-state Li-ion batteries, etc. ).
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高影响因子
Advanced Energy Materials
·
2024
·Vol. 14
·期 36
·2401509
·
IF 24.4
Han Yu,Guoliang Zhang,Dongmei Zhang,Ruonan Yang,Xia Li,Xiuqi Zhang,Gang Lian,Hua Hou,Zhanhu Guo,Chuanxin Hou,Xiaoyang Yang,Feng Dang
Although lithium–oxygen batteries (LOBs) hold great promise as future energy storage systems, they are impeded by insulated discharge product Li 2 O 2 and sluggish oxygen reduction reaction/oxygen evolution revolution (ORR/OER) kinetics. The application of a highly efficient cathode catalyst determines the LOBs performance. The d-band modulation and catalytic kinetics promotion are important concept guidelines for the performance enhancement of cathode catalysts. In this work, the homogeneous in-plane distortion-derived synergistic catalytic capability of an Ag 2 Mo 2 O 7 catalyst with modulated d-band centers and promoted ORR/OER kinetics is demontrated. The uniform elongation of Ag─O bonds and compression of Mo─O bonds in (020) plane leads to d-band splitting and d-band center optimization and delivers improved adsorption behavior for high ORR/OER capability. Furthermore, the spatial and energy overlap of Ag d xz and O 2 anti-bonding π * orbitals facilitate electron injection during ORR process and reduce the energy barrier for charge transfer and O 2 desorption during OER process, accelerating the ORR/OER kinetics. As a result, the (020) plane-exposed Ag 2 Mo 2 O 7 cathode exhibits ultralong cycle stability of 817 cycles at 500 mA g −1 and large specific discharge/charge capacities of 15898/15180 mAh g −1 . This work provides facile concept guidance for optimizing catalytic capability through controlled lattice distortion in cathode catalysts for LOBs.
研究领域:
材料科学
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电化学
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能量存储
·
催化
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DOI
高影响因子
ANALYTICAL CHEMISTRY
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2014
·
IF 5.825
Chuantao Hou,Dapeng Yang,Bo Liang,Aihua Liu
The power output and stability of enzyme-based biofuel cells (BFCs) is greatly dependent on the properties of both the biocathode and bioanode, which may be adapted for portable power production. In this paper, a novel highly uniform three-dimensional (3D) macroporous gold (MP-Au) film was prepared by heating the gold “supraspheres”, which were synthesized by a bottom-up protein templating approach, and followed by modification of laccase on the MP-Au film by covalent immobilization. The as-prepared laccase/MP-Au biocathode exihibited an onset potential of 0.62 V versus saturated calomel electrode (SCE, or 0.86 V vs NHE, normal hydrogen electrode) toward O2 reduction and a high catalytic current of 0.61 mAcm–2. On the other hand, mutated glucose dehydrogenase (GDH) surface displayed bacteria (GDH-bacteria) were used to improve the stability of the glucose oxidation at the bioanode. The as-assembled membraneless glucose/O2 fuel cell showed a high power output of 55.8 ± 2.0 μW cm–2 and open circuit potential of 0.80 V, contributing to the improved electrocatalysis toward O2 reduction at the laccase/MP-Au biocathode. Moreover, the BFC retained 84% of its maximal power density even after continuous operation for 55 h because of the high stability of the bacterial surface displayed GDH mutant toward glucose oxidation. Our findings may be promising for the development of more efficient glucose BFC for portable battery or self-powered device applications.
研究领域:
生物化学
·
材料科学
·
能源技术
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产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Yuanhong Xie,Chenrui Liu,Dejian Li,Yun Liu
Herein, a novel composite of MIL-101(Fe) loaded with nitrogen doped carbon quantum dots (NCQDs/MIL-101(Fe), denoted as NQML), which can construct dual effect of photocatalysis and photo-Fenton for organic pollutants removal, was prepared by solvent impregnation method. Characterization methods proved that NQML had been synthesized successfully. Additionally, the adding volume of NCQDs could effectively influence the photocatalytic activities of NQML-x composites (x represents the adding volume of NCQDs) for tetracycline (TC) degradation, and NQML-8 exhibited the optimum photocatalytic performance among the studied catalysts upon visible light illumination under natural pH, which can completely degrade TC within 180 min. By comparison, the TC degradation kinetic constant in the system with NQML-8 was as 15.85 and 8.24 folds of that in the NCQDs and MIL-101(Fe) systems, respectively. The mechanism study proved that the enhanced photocatalytic performance of NQML was resulted from the visible light up-conversion property, electron-hole separation and transfer capacity of NCQDs. Meanwhile, NQML could not only produce h + but also lead to in-situ generation of O 2 - and H 2 O 2 by activation of O 2 under visible light. The generated H 2 O 2 could react with Fe(II) in MIL-101(Fe) to produce OH so as to construct a dual effect of photocatalysis and photo-Fenton in TC removal.
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DOI
高影响因子
CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Taoyi Lu,Xingmin Feng,Zhiqin Wen,Li Tang,Suzhen Kang,Jiyuan Huang,Gaoxiang Wei,Siyi Huang,Defeng Long,Sheng Wang
In this study, (Ce 0.2 Zr 0.2 La 0.2 Yb 0.2 Ln 0.2 )O 2- δ (Ln = Er, Y, Sm; labelled as H-Er, H-Y, H-Sm) high-entropy fluorite oxides (HEFOs) are designed by standard deviation and first-principles calculation. These HEFOs are subsequently synthesized via solid-phase reaction method, and the phase formation, microstructure, mechanical and thermal properties of the three samples have been systematically investigated. The results show that the three samples, exhibiting a single-phase fluorite structure, are successfully prepared after sintering at 1600 °C, and all the elements are uniformly distributed with no elemental segregation and agglomeration. The calculated δ of H-Er, H-Y and H-Sm are 0.3399, 0.3668 and 0.3458, respectively, so the chemical formula of three HEFOs are (Ce 0.2 Zr 0.2 La 0.2 Yb 0.2 Er 0.2 )O 1.6601 , (Ce 0.2 Zr 0.2 La 0.2 Yb 0.2 Y 0.2 )O 1.6332 and (Ce 0.2 Zr 0.2 La 0.2 Yb 0.2 Sm 0.2 )O 1.6542 , respectively. Additionally, the effects of rare earth ions (Er, Y and Sm) on the hardness, Young's modulus and thermal conductivity of HEFOs are analyzed. H-Y exhibits the highest hardness value and largest Young's modulus among the three HEFOs, primarily due to the largest mean acoustic velocity and cohesion energy in absolute value, smallest AGS and average bond lengths. The thermal conductivities ( κ ) of the three samples are only 1.465–1.598 W m −1 K −1 at 1000 °C. Furthermore, the thermal conductivities of the three samples are significantly lower than that of 8YSZ within the temperature range from 25 °C to 1000 °C, and H-Sm exhibits the lowest thermal conductivity in this temperature range. Consequently, they are anticipated to have promising applications in the field of thermal barrier coatings (TBCs).
研究领域:
材料科学
·
固体力学
·
计算材料学
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产品关联
DOI
高影响因子
Energy Storage Materials
·
2025
·
IF 20.2
Yuzhen Dang,Yurong Wu,Zhe Xu,Runguo Zheng,Zhiyuan Wang,Xiaoping Lin,Yanguo Liu,Sha Liu,Leijie Zhang,Dan Wang
P2-type manganese-based cathode materials are notable for their high theoretical capacity and open prismatic channels. However, rapid capacity decay caused by harmful irreversible phase transformations (P2-O2) and oxygen release in the high-voltage region (>4.2 V) limits their commercial application. Here, a co-doping strategy with lithium and niobium is proposed to enhance the structural stability at both room-temperature (RT) and low-temperature (LT) over extended cycles. The X-ray absorption near-edge spectra and first-principles calculations reveal that Li doping elevates the valence states of transition metals, thereby enhancing the reversibility of anionic redox reactions. Additionally, Nb doping leads to the formation of a rock-salt-like phase on the surface, which improves the stability of the electrode/electrolyte interface. In situ X-ray diffraction and differential electrochemical mass spectrometry show that Li and Nb co-doping prevents the P2-O2 phase transition, suppresses gas release, and enhances long-cycle stability. The P2-Na 0.67 Ni 0.24 Mn 0.64 Li 0.1 Nb 0.02 O 2 (NNMLNb) exhibits a reversible specific capacity of 127.4 mAh g −1 and 101.5 mAh g −1 at -20 °C and -30 °C, respectively. Remarkably, the sample cycles stably for 1200 cycles with a discharge capacity of 85 mAh g −1 , corresponding 90 % capacity retention. This work provides a novel strategy to improve the cycling life of sodium-ion batteries at both RT and LT.
研究领域:
能源材料
·
电化学
·
电池技术
·
材料科学
·
固态化学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）