International Journal of Nanomedicine
·
2024
·
IF 6.6
Dan Wang,Xiaobo Wang,Yan Li,Xiaowei Wang,Xuelei Wang,Jiayi Su,Apeng Wang,Kai Lv,Mingliang Liu,Guimin Xia
Background Gemcitabine (Gem) is one of the first-line chemotherapy drugs for pancreatic cancer treatment. However, its short half-life in plasma and adverse effects limited its broader application.Methods A novel Gem derivative (N4-tetradecyloxycarbonyl gemcitabine, tcGem) was synthesized and encapsulated into liposomes (LipotcGem) to overcome the above shortcomings.Results LipotcGem has been successfully formulated, with the average size of 115 nm, zeta potential values of −36 mV, encapsulation efficiency of up to 98%, and drug loading capacity of 8.1%. Compared to Gem, LipotcGem improved in vitro antitumor activity significantly, as evidenced by the lower IC50, the higher percentage of apoptotic cells, the stronger ability to inhibit cell migration and invasion due to the higher cellular accumulation (100 times). Additionally, the endocytosis of LipotcGem was mainly mediated by caveolae, and was then processed in the lysosome, where tcGem was released and hydrolyzed into Gem. LipotcGem inhibited tumor growth by 70% in subcutaneous xenograft model and 90% in orthotopic xenograft model, respectively. LipotcGem suppressed tumor metastasis and prolonged survival without perceptible systemic toxicity, which may be caused by the longer t1/2 in vivo (3.5 times, 5.23 vs 1.46 h) and more enrichment in tumor tissue (750 times).Conclusion LipotcGem significantly increased the anti-tumor efficiency and decreased the toxicity for chemotherapy of pancreatic cancer.
研究领域:
肿瘤学
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药学
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药物递送系统
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癌症研究
✓ 已验证
产品关联
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.
研究领域:
材料科学
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电化学
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催化科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Chunfeng Shao,Lingmin Wu,Yinghua Wang,Konggang Qu,Hailiang Chu,Lixian Sun,Jianshan Ye,Baitao Li,Xiujun Wang
Single-atom catalysts (SACs) have sparked intense interest in heterogeneous catalysis lately, but insufficient accessibility of active sites restricts their further applications. Herein, a hydrangea-like carbon nanoparticle possessing highly open nanospaces and enhanced external surface area that fully exposes the catalytic sites is reported. By introducing mesoporous silica nanoparticles (MSNs), Fe-doping zeolitic imidazolate framework-8 (ZIF-8) precursors are assembled into a flower-like superstructure interlaced by porous nanosheets, which expand from inside out constructing an open and interconnected architecture. This unique structure can substantially liberate the densely dispersed but deeply buried Fe-N 4 sites inside carbon nanoparticles and accelerate mass transfer in the catalyst layer that increases active-site utilization. Furthermore, the physical and chemical properties of the assembled catalysts can be adjusted by the diameter (200, 300, and 500 nm) of MSNs. When the diameter was 500 nm, the optimal FeNC-F3 catalyst exhibited large specific surface area, maximum metal centers utilization, high oxygen reduction reaction efficiency, and excellent stability. The novel cathodic electrocatalyst achieved high power density of 0.32 mW cm −2 in microbial fuel cell and 288 mW cm −2 in Zn-air battery. This work established a realistic strategy for promoting the practical development of fuel cell catalysts.
研究领域:
材料科学
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电化学
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催化
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能源存储与转换
✓ 已验证
产品关联
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2024
·
IF 8.2
Tao Ai,Siyu Yao,Yuanyuan Yu,Kai Peng,Ling Jin,Xifen Zhu,Haijun Zhou,Jiahui Huang,Jianteng Sun,Lizhong Zhu
Sulfonamide antibiotics, extensively used in human and veterinary therapy, accumulate in agroecosystem soils through livestock manure and sewage irrigation. However, the interaction between sulfonamides and rice plants remains unclear. This study investigated the transformation behavior and toxicity of sulfamethoxazole (SMX) and its main metabolite, N4-acetyl-sulfamethoxazole (NASMX) in rice. SMX and NASMX were rapidly taken up by roots and translocated acropetally. NASMX showed higher accumulating capacity, with NASMX concentrations up to 20.36 ± 1.98 μg/g (roots) and 5.62 ± 1.17 μg/g (shoots), and with SMX concentrations up to 15.97 ± 2.53 μg/g (roots) and 3.22 ± 0.789 μg/g (shoots). A total of 18 intermediate transformation products of SMX were identified by nontarget screening using Orbitrap-HRMS, revealing pathways such as deamination, hydroxylation, acetylation, formylation, and glycosylation. Notably, NASMX transformed back into SMX in rice, a novel finding. Transcriptomic analysis highlights the involvements of cytochrome P450 (CYP450), acetyltransferase (ACEs) and glycosyltransferases (GTs) in these biotransformation pathways. Moreover, exposure to SMX and NASMX disrupts TCA cycle, amino acid, linoleic acid, nucleotide metabolism, and phenylpropanoid biosynthesis pathways of rice, with NASMX exerting a stronger impact on metabolic networks. These findings elucidate the sulfonamides' metabolism, phytotoxicity mechanisms, and contribute to assessing food safety and human exposure risk amid antibiotic pollution.
研究领域:
环境科学
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植物生理学
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药理学
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分子生物学
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毒理学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2024
·Vol. 27
·期 24
·e202400196
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IF 2.2
Wenkang Mao,Jinjing Ju,Dan Li,Daishe Wu,Feigao Xu
Graphical Synopsis: A pyrrolic N-rich g-C 3 N 4 (PN-g-C 3 N 4 ) framework is synthesized with transition metal M (M=Fe, Co, Ni, Cu, Cr, and Mn) atomic sites coordinated onto it. M/PN-g-C 3 N 4 are constructed for peroxodisulfate activation. The synergy between photocatalysis and Fe/PN-g-C 3 N 4 catalyst results in increased generation and separation of charge carriers, along with the cyclic transformation of the Fe 3+ /Fe 2+ couple. Photocatalysis is an efficient technology for the degradation of pollutants. However, there is still much room for improvement in its degradation efficiency. In this study, a pyrrolic N-rich g-C 3 N 4 (PN-g-C 3 N 4 ) framework was synthesized with transition metal M (M=Fe, Co, Ni, Cu, Cr, and Mn) atomic sites coordinated onto it. Then, a series of single atomic metals M anchored to PN-g-C 3 N 4 (M/PN-g-C 3 N 4 ) are constructed for peroxodisulfate activation. Their order of catalytic activity follows Fe>Cr>Ni>Cu≈Co>Mn, in particular the degradation rates of the TCH for Fe-PN-g-C 3 N 4 are 3.74 times higher than that of undoped PN-g-C 3 N 4 . These carefully regulated pyrrolic N-rich Fe sites demonstrate outstanding performance in degrading organic pollutant. As an exemplary model, the Fe/PN-g-C 3 N 4 catalyst efficiently drives the catalytic oxidation of TCH through Fenton-like reaction under visible light, showcasing exceptional cycle stability and a broad effective pH range of 3.0–11.0. The synergy between photocatalysis and Fe doped catalysis results in increased generation and separation of charge carriers, along with the cyclic transformation of the Fe 3+ /Fe 2+ couple. This combination significantly enhances the Fenton-like performance, making it a highly effective process for pollutant degradation.
研究领域:
环境科学
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催化
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材料科学
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化学工程
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水处理技术
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 19
·11792-11801
·
IF 10.733
Xiang Ao,Wei Zhang,Zhishan Li,Lin Lv,Yunjun Ruan,Hong-Hui Wu,Wei-Hung Chiang,Chundong Wang,Meilin Liu,Xiao Cheng Zeng
The scarcity and weak durability of precious metal catalysts are among the biggest obstacles to achieving cost-effective electrocatalysts in fuel cells and metal–air batteries. Hence, it is imperative to develop low-cost non-precious metal catalysts with comparable oxygen reduction reaction (ORR) activity to precious metal catalysts. Herein, we report a highly effective strategy for the facile synthesis of Fe/N-functionalized 3D porous carbon networks. A major advantage of the newly designed catalyst is that ultrafine Fe4N nanoparticles are grown and uniformly mounted on the carbon framework upon pyrolysis treatment at 800 °C, and co-exist with numerous in situ formed Fe–N4 moieties in the carbon matrix, being evidenced by using X-ray absorption and photoelectron spectroscopy. The new electrocatalysts exhibit high ORR activity, comparable/superior to that of the state-of-the-art Fe/N–carbon based catalysts reported to date. Specifically, the catalysts show a half-wave potential of 0.890 V (vs. RHE) and a limited current density of 6.18 mA cm−2. By resorting to experimental measurements and density-functional theory (DFT) calculations, the synergistic effects between Fe–N4 moieties and the Fe4N support are identified for the first time, which play a key role in boosting the catalytic performance of the Fe/N-functionalized porous carbon networks.
研究领域:
材料科学
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电化学
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催化
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能源材料
✓ 已验证
产品关联
DOI
高影响因子
Research
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2023
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IF 11
Guangchun Song,Jia Xu,Hong Zhong,Qi Zhang,Xin Wang,Yitong Lin,Scott P. Beckman,Yunbo Luo,Xiaoyun He,Jin-Cheng Li,Kunlun Huang,Nan Cheng
The enzyme-mimicking catalytic activity of single-atom nanozymes has been widely used in tumor treatment. However, research on alleviating metabolic diseases, such as hyperglycemia, has not been reported. Herein, we found that the single-atom Ce-N4-C-(OH)2 (SACe-N4-C-(OH)2) nanozyme promoted glucose absorption in lysosomes, resulting in increased reactive oxygen species production in HepG2 cells. Furthermore, the SACe-N4-C-(OH)2 nanozyme initiated a cascade reaction involving superoxide dismutase-, oxidase-, catalase-, and peroxidase-like activity to overcome the limitations associated with the substrate and produce •OH, thus improving glucose intolerance and insulin resistance by increasing the phosphorylation of protein kinase B and glycogen synthase kinase 3β, and the expression of glycogen synthase, promoting glycogen synthesis to improve glucose intolerance and insulin resistance in high-fat diet-induced hyperglycemic mice. Altogether, these results demonstrated that the novel nanozyme SACe-N4-C-(OH)2 alleviated the effects of hyperglycemia without evident toxicity, demonstrating its excellent clinical application potential.
研究领域:
纳米技术
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生物化学
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代谢疾病
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药理学
✓ 已验证
DOI
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.
研究领域:
材料科学
·
电化学
·
能源存储与转换
✓ 已验证
产品关联
DOI
高影响因子
Science Bulletin
·
2025
·
IF 21.1
Ergui Luo,Jingyi Liang,Kexuan Zhang,Xian Wang,Luozhen Jiang,Tianjun Hu,Junming Zhang,Junjie Ge,Jianfeng Jia
Electrochemical two-electron oxygen reduction reaction (2e − ORR) serves as an appealing approach for green hydrogen peroxide (H 2 O 2 ) production. However, the corresponding progress in efficient non-precious metal catalysts for acidic 2e − ORR has not kept pace, with the research model being almost confined to Co-based system. Here, guided by molecular dynamics simulations, the active nature and origin of pyrolyzed Cr−N 4 catalysts for ORR are unveiled, wherein the over-strong oxygen affinity of the Cr center is counterbalanced by a spontaneous axial O-coordination. By creating an oxidation-induced electron-deficient environment, the Cr−N 4 can be flexibly tailored for selective H 2 O 2 formation. A single-atom Cr−N 4 /C(O) catalyst is developed experimentally, which rivals and even slightly outperforms its Co-based counterpart in terms of selectivity (92% versus 71%) and productivity (202 versus 145 mmol g cat −1 h −1 ) for H 2 O 2 . More encouragingly, the Cr-based catalysts exhibit minimal reactivity towards H 2 O 2 -related side reactions, with the metal component being robust against leaching. This research marks the first identification of pyrolyzed Cr−N 4 catalysts as competent for acidic two-electron O 2 reduction to H 2 O 2 . The innovative models and insights offer profound guidance for the design of future-generation catalysts for electrochemical H 2 O 2 synthesis.
研究领域:
电催化
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材料科学
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能源化学
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可持续化学
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计算化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Small
·
2023
·Vol. 19
·期 33
·2301391
·
IF 13.3
Wenjing Zhang,Jian Zheng,Ruoyu Wang,Li Huang,Junkai Wang,Tianran Zhang,Xiangfeng Liu
Lithium–oxygen (Li–O 2 ) batteries have received extensive attention owing to ultrahigh theoretical energy density. Compared to typical discharge product Li 2 O 2 , LiOH has attracted much attention for its better chemical and electrochemical stability. Large-scale applications of Li–O 2 batteries with LiOH chemistry are hampered by the serious internal shuttling of the water additives with the desired 4e − electrochemical reactions. Here, a metal organic framework-derived “water-trapping” single-atom-Co-N 4 /graphene catalyst (Co-SA-rGO) is provided that successfully mitigates the water shuttling and enables the direct 4e − catalytic reaction of LiOH in the aprotic Li–O 2 battery. The Co-N 4 center is more active toward proton-coupled electron transfer, benefiting - direction 4e − formation of LiOH. 3D interlinked networks also provide large surface area and mesoporous structures to trap ≈12 wt% H 2 O molecules and offer rapid tunnels for O 2 diffusion and Li + transportation. With these unique features, the Co-SA-rGO based Li–O 2 battery delivers a high discharge platform of 2.83 V and a large discharge capacity of 12 760.8 mAh g −1 . Also, the battery can withstand corrosion in the air and maintain a stable discharge platform for 220 cycles. This work points out the direction of enhanced electron/proton transfer for the single-atom catalyst design in Li–O 2 batteries.
研究领域:
材料科学
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电化学
·
能源存储
·
电池技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 8
·4369-4375
·
IF 11.301
Lulu Chen,Yelong Zhang,Lile Dong,Wenxiu Yang,Xiangjian Liu,Ling Long,Changyu Liu,Shaojun Dong,Jianbo Jia
Rational design of isolated metal atom doped carbon catalysts is essential for revealing the essence of high activity for the oxygen reduction reaction (ORR), which can promote the development of robust catalysts for clean energy conversion devices. Herein, we report a simple one-step strategy to prepare Fe and Co atomically supported on N-doped nanocarbon (FeCo-IA/NC) from metal–organic frameworks with excellent ORR activity. The isolated Fe–N4 and Co–N4 sites are characterized by atomic-resolution aberration-corrected scanning transmission electron microscopy and X-ray absorption fine structure spectroscopy. The electrochemical results and density functional theory calculations indicate that the synergetic effect between Fe–N4 and Co–N4 accounts for the enhanced ORR activity. Benefiting from the large BET surface area, microporous feature, and high content (85%) of pyridinic and graphitic N, the well-designed catalyst exhibits better ORR activity (half-wave potential of 0.88 V) and Zn–air battery performances (higher open circuit potential and power density) than commercial Pt/C. This work may lay a foundation for further exploring efficient non-precious metal-based catalysts for the ORR and developing clean energy conversion devices.
研究领域:
材料科学
·
电化学
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED MATERIALS
·
2021
·Vol. 34
·期 5
·2105410
·
IF 30.849
Leping Yang,Xu Zhang,Lingxiao Yu,Jianhua Hou,Zhen Zhou,Ruitao Lv
Noble-metal-free, durable, and high-efficiency electrocatalysts for oxygen reduction and evolution reaction (ORR/OER) are vital for rechargeable Zn–air batteries (ZABs). Herein, a flexible and free-standing carbon fiber membrane immobilized with atomically dispersed Fe–N 4 /C catalysts (Fe/SNCFs-NH 3 ) is synthesized and used as air cathode for ZABs. The intertwined fibers with hierarchical nanopores facilitate the gas transportation, electrolyte infiltration and electron transfer. The large specific surface area exposes a high concentration of Fe–N 4 /C sites embedded in the carbon matrix. Modulation of local atomic configurations by sulfur doping in Fe/SNCFs-NH 3 catalyst leads to excellent ORR and enhanced OER activities. The as-synthesized Fe/SNCFs-NH 3 catalyst demonstrates a positive half-wave potential of 0.89 V and a small Tafel slope of 70.82 mV dec –1 , outperforming the commercial Pt/C (0.86 V/94.74 mV dec –1 ) and most reported M–N x /C (M = Fe, Co, Ni) catalysts. Experimental characterizations and theoretical calculations uncover the crucial role of S doping in regulating ORR and OER activities. The liquid-state ZABs with Fe/SNCFs-NH 3 catalyst as air cathode deliver a large peak power density of 255.84 mW cm –2 and long-term cycle durability over 1000 h. Solid-state ZAB shows stable cycling at various flat/bent/flat states, demonstrating great prospects in flexible electronic device applications.
研究领域:
材料科学
·
电化学
·
能源存储
·
电池技术
·
催化
✓ 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）