SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Xin Li,Wanrong Bu,Ke Zhu,Yuwen Chen,Xiaoying Liang,Bin Wang,Yuchen Wang,Kai Yan
Single-atom catalysts (SACs) as photo-Fenton-like catalysts have attracted widespread attention in water purification. However, the development of SACs with renewability, cleanliness, high mass loading, and raw material abundance is a formidable challenge to achieve efficient pollutant removal. In this study, we fabricated high-performance Fe-nanocluster embedded biomass-derived carbon (Fe/Bio-C) from Ficus altissima wastes for quinolone antibiotics degradation. The high-angle annular dark-field scanning transmission electron microscopy with aberration correction (AC-HAADF-STEM) and X-ray absorption fine structure spectroscopy (XAFS) revealed that the Fe/Bio-C exhibited a porous structure with abundant Fe-N 4 active sites. The Fe/Bio-C catalysts achieved an exceptional efficiency of 98.6 % for the removal of the representative quinolone antibiotic, namely lomefloxacin (LOM), within 30 min. Furthermore, an in-depth exploration was conducted to assess the influence of reaction parameters on degradation performance, kinetics, toxicity, and mechanism. The free radical quenching experiments and electron paramagnetic resonance (EPR) spectra demonstrated the existence of ·O 2 − , 1 O 2 , ·OH, SO 4 · − in the reaction system and the ·O 2 − radicals played a relatively important role in the degradation progress. This work broaden the avenue for constructing metal-nanocluster photocatalysts with the high reactivity, low metal leaching, and universality to various pollutants.
研究领域:
环境科学
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材料科学
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化学工程
·
水处理
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DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-10
·
IF 14.7
Yin Shuhu,Chen Long,Yang Jian,Cheng Xiaoyang,Zeng Hongbin,Hong Yuhao,Huang Huan,Kuai Xiaoxiao,Lin Yangu,Huang Rui,Jiang Yanxia,Sun Shigang
Replacement of expensive and rare platinum with metal–nitrogen–carbon catalysts for oxygen reduction reactions in proton exchange membrane fuel cells is hindered by their inferior activity. Herein, we report a highly active iron-nitrogen-carbon catalyst by optimizing the carbon structure and coordination environments of Fe-N 4 sites. A critical high-temperature treatment with ammonium chloride and ammonium bromide not only enhances the intrinsic activity and density of Fe-N 4 sites, but also introduces numerous defects, trace Br ions and creates mesopores in the carbon framework. Notably, surface Br ions significantly improve the interaction between the ionomer and catalyst particles, promoting ionomer infiltration and optimizing the O 2 transport and charge transfer at triple-phase boundary. This catalyst delivers a high peak power density of 1.86 W cm −2 and 54 mA cm −2 at 0.9 V iR-free in a H 2 -O 2 fuel cells at 80 °C. Our findings highlight the critical role of interface microenvironment regulation.
研究领域:
电化学
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催化
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能源材料
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燃料电池
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DOI
PubMed
高影响因子
ACS Nano
·
2024
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IF 15.8
Xuelei Wang,Xiaowei Wang,Jiayi Su,Dan Wang,Wenkai Feng,Xiaobo Wang,Hongwei Lu,Apeng Wang,Mingliang Liu,Guimin Xia
Acute myeloid leukemia (AML) is a hematological malignancy with a high recurrence rate. The interaction of chemokine receptor 4/chemokine ligand 12 (CXCR4/CXCL12) mediates homing and adhesion of AML cells in bone marrow, leading to minimal residual disease in patients, which brings a hidden danger for future AML recurrence. Ara-C is a nonselective chemotherapeutic agent against AML. Due to its short half-life and severe side effects, a lipid-like Ara-C derivative (AraN) was synthesized and a dual-function LipoAraN-E5 (135 nm, encapsulation efficiency 99%) was developed, which coloaded AraN and E5, a peptide of the CXCR4 antagonist. LipoAraN-E5 effectively improved the uptake, enhanced the inhibition of leukemia cell proliferation, migration, and adhesion to stromal cells in bone marrow, and mobilized the leukemia cells from bone marrow to peripheral blood via interfering with the CXCR4/CXCL12 axis. LipoAraN-E5 prolonged the plasma half-life of AraN (8.31 vs 0.56 h) and was highly enriched in peripheral blood (3.67 vs 0.05 μmol/g at 8 h) and bone marrow (379 vs 148 μmol/g at 24 h). LipoAraN-E5 effectively prevented the infiltration of leukemia cells in peripheral blood, bone marrow, spleen, and liver, prolonged the mice survival, and showed outstanding antineoplastic efficacy with negligible toxicity, which were attributed to the ingenious design of AraN, the use of a liposomal delivery carrier, and the introduction of E5. Our work revealed that LipoAraN-E5 may be a promising nanocandidate against AML.
研究领域:
肿瘤学
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药理学
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血液学
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DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Cheng Gao,Longzhu Li,Xiaoming Yan,Ning Zhang,Junjiang Bao,Xiaopeng Zhang,Yanqiang Li
Transition metal single atom catalysts (TM SACs) are the most promising oxygen reduction reaction (ORR) catalysts for proton exchange membrane fuel cells (PEMFCs) and metal-air batteries. However, the low density of M-N x active sites seriously hinders further improvement of the ORR electrocatalytic activity. Here, a strategy for encapsulating nitrogen-rich guest molecules (triethylenediamine cobalt complex, [Co(en) 3 ] 3+ ) was proposed to construct a high-performance cobalt single-atom catalyst (Co-encapsulated SAC/NC). With this strategy, the guest molecules are encapsulated into metal–organic framework (MOF) cages as an additional cobalt source to boost cobalt loading, while abundant nitrogen from guest molecules contributes to the formation of Co-N 4 active sites. Remarkably, the resulting Co-encapsulated SAC/NC has a high cobalt loading amount of 4.03 wt%, and spherical aberration-corrected transmission electron microscopy (AC-TEM) has confirmed that most cobalt exists in a single-atom state. As a result, the Co-encapsulated SAC/NC exhibits excellent ORR catalytic performance with a half-wave potential of 0.88 V. Furthermore, Zn-air batteries employing Co-encapsulated SAC/NC as air cathode show high peak power density and excellent cycling stability. Density functional theory (DFT) calculations reveal that adjacent active sites have different rate-determining steps and lower reaction energy barriers than a single active site.
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产品关联
DOI
PubMed
高影响因子
Advanced Energy Materials
·
2023
·Vol. 13
·期 22
·2300325
·
IF 27.8
Zhen Zhang,Tianping Wang,Weiwen Wang,Xiangnan Wang,Xianglin Luo,Chong Cheng,Xikui Liu
Metallophthalocyanines (MPcs) hold great promise in the electrochemical reduction of oxygen; however, their practical applications in energy storage and conversion are still limited by their low stability and poor water oxidation activity. Herein, a novel stable 2D imide-linked metalphthalocyanine framework (denoted as FePc-PI) is reported, that has atomically dispersed Fe-N 4 sites deposited on the KB substrate via in situ growth, followed by incorporation of ultrafine nickel oxide nanoparticles (NiO x @FePc-PI/KB) to induce bifunctional electrocatalytic activities for the oxygen reduction reaction and oxygen evolution reaction. Benefitting from the robust aromatic backbone, the engineered catalytic centers, and the unique electronic structures owing to the interaction between the Fe-N 4 sites and NiO x species, the newly developed NiO x @FePc-PI/KB catalyst exhibits excellent reversible oxygen bifunctional activity ( E 1/2 = 0.926 V, η 10 = 285 mV), delivering a record-low overpotential difference (Δ E ) of 0.59 V, which far exceeds the noble-metal-based Pt/C+RuO 2 benchmark (Δ E = 0.77 V) and represents the highest level for reported bifunctional electrocatalysts. Furthermore, the rechargeable aqueous Zn-air batteries assembled with the NiO x @FePc-PI/KB catalyst deliver a high peak power density of 232.9 mW cm −2 and long-term cycling durability over 1400 cycles. Flexible all-solid-state Zn-air batteries exhibit stable cycling at various flat/bent/flat states, thus demonstrating their excellent prospects in realistic implementations.
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Qiaoqiao Mu,Wei Zhu,Xian Li,Chufeng Zhang,Yanhui Su,Yuebin Lian,Pengwei Qi,Zhao Deng,Duo Zhang,Shuao Wang,Xing Zhu,Yang Peng
In this work, composite thin films comprising the 2D/2D MOF/rGO heterostructures assembled via Coulomb interaction are employed as the cocatalyst for photocatalytic CO 2 reduction for the first time. The electrostatic charge transfer and the strong π-π interaction induced in the heterostructure effectively modulate the electronic structure of the metal centers in the conductive 2D MOF (Ni 3 HITP 2 ), evidenced by Zeta Potentials, HR-TEM, XPS and XANES. The best thin-film catalyst with an optimal MOF/rGO ratio demonstrates a high CO evolution rate of 3.8 × 10 4 μmol h −1 g film −1 (0.46 min −1 in TOF) and a good selectivity of 91.74%, synergically contributed by the improved photoelectron harvesting on the rGO scaffold, the efficient charge transportation/transfer within the conductive and intimate 2D heterostructure, the coherent energy flow owing to aligned energy levels, and the enriched electron density at the isolated Ni-N 4 sites boosted by electrostatic charge transfer.
研究领域:
材料科学
·
催化
·
光化学
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纳米技术
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环境科学
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DOI
高影响因子
危险品化学品经营许可证（带存储）