Theranostics
·
2022
·
IF 11.6
Qiqi Xu,Yuetong Zhang,Zulu Yang,Guohui Jiang,Mingzhu Lv,Huan Wang,Chenghui Liu,Jiani Xie,Chengyan Wang,Kun Guo,Zhanjun Gu,Yuan Yong
Nanozyme-based tumor collaborative catalytic therapy has attracted a great deal of attention in recent years. However, their cooperative outcome remains a great challenge due to the unique characteristics of tumor microenvironment (TME), such as insufficient endogenous hydrogen peroxide (H 2 O 2 ) level, hypoxia, and overexpressed intracellular glutathione (GSH). Methods: Herein, a TME-activated atomic-level engineered PtN 4 C single-atom nanozyme (PtN 4 C-SAzyme) is fabricated to induce the “butterfly effect” of reactive oxygen species (ROS) through facilitating intracellular H 2 O 2 cycle accumulation and GSH deprivation as well as X-ray deposition for ROS-involving CDT and O 2 -dependent chemoradiotherapy. Results: In the paradigm, the SAzyme could boost substantial ∙OH generation by their admirable peroxidase-like activity as well as X-ray deposition capacity. Simultaneously, O 2 self-sufficiency, GSH elimination and elevated Pt 2+ release can be achieved through the self-cyclic valence alteration of Pt (IV) and Pt (II) for alleviating tumor hypoxia, overwhelming the anti-oxidation defense effect and overcoming drug-resistance. More importantly, the PtN 4 C-SAzyme could also convert O 2 ·- into H 2 O 2 by their superior superoxide dismutase-like activity and achieve the sustainable replenishment of endogenous H 2 O 2 , and H 2 O 2 can further react with the PtN 4 C-SAzyme for realizing the cyclic accumulation of ∙OH and O 2 at tumor site, thereby generating a “key” to unlock the multi enzymes-like properties of SAzymes for tumor-specific self-reinforcing CDT and chemoradiotherapy. Conclusions: This work not only provides a promising TME-activated SAzyme-based paradigm with H 2 O 2 self-supplement and O 2 -evolving capacity for intensive CDT and chemoradiotherapy but also opens new horizons for the construction and tumor catalytic therapy of other SAzymes.
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高影响因子
CORROSION SCIENCE
·
2020
·
IF 6.479
Junying Hu,Qi Xiong,Longjun Chen,Chenfeng Zhang,Ziqi Zheng,Shuai Geng,Zhi Yang,Xiankang Zhong
The corrosion inhibition of carbon steel in CO 2 -O 2 -containing environment is one of the biggest challenges in flue gas injection for enhanced oil recovery. Herein we report the possibility to use Bis(2-ehylhexyl) phosphate (BEP) to inhibit the corrosion in CO 2 -O 2 -containing solution and simultaneously the inhibition mechanisms are unmasked. The results show that the corrosion is greatly inhibited with 500 ppm BEP in 1 wt% NaCl solution with 0.02 MPa CO 2 and 3 mg/L O 2 . BEP could interact with Fe and corrosion products via the formation of P-O-Fe bond and P-Fe bond to generate a barrier layer, thus, offering a protective performance.
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BIOCONJUGATE CHEMISTRY
·
2021
·
IF 4.774
Chunxiao Sui,Rui Tan,Yiwen Chen,Guotao Yin,Ziyang Wang,Wengui Xu,Xiaofeng Li
Metal–organic frameworks (MOFs) derivatives had been widely explored in electronic and environmental fields, but rarely evaluated in the biomedical applications. Herein, Fe–N codoped carbon (FeNC) nanoparticles were synthesized and characterized via facile pyrolysis of precursor ZIF-8 (Fe/Zn) nanoparticles, and their potential applications in tumor therapy were assessed in this investigation both in vitro and in vivo. After PAA (sodium polyacrylate) modification, the FeNC@PAA nanoparticles were able to initiate a Fe-based Fenton-like reaction to generate ·OH and O2 for chemodynamic therapy (CDT) and O2 evolution. Meanwhile, the porphyrin-like metal center in the FeNC@PAA nanoparticles could be used as a photosensitizer for photodynamic therapy (PDT) of tumors, which could be enhanced by O2 generated in CDT. Furthermore, the FeNC@PAA nanoparticles were also found to be effective in photothermal therapy (PTT) with a photothermal conversion efficiency of 29.15%, owing to a high absorbance in the near-infrared region (NIR). In conclusion, the synthesized FeNC@PAA nanoparticles exhibited promising applications in O2 evolution and CDT/PDT/PTT synergistic treatment of tumors.
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高影响因子
JOURNAL OF POWER SOURCES
·
2020
·
IF 8.247
Ying Wang,Dan Li,Siqi Zhang,Ziye Kang,Haiming Xie,Jia Liu
Although dual redox mediators (RMs) largely promote the discharge capacity and decreases the charge overpotential in Li-O 2 batteries , the shuttle effect leads to a RM degradation and a serious deterioration of Li metal, which results in a poor sustainability. Here, a poly (3,4-ethylenedioxythiophene):poly (styrenesulfonate) (PEDOT:PSS) -decorated separator has been firstly introduced into a dual mixture RMs-involved Li-O 2 system, which restrains the shuttle effect via coulombic interactions. Benefiting from the advantages of as-prepared separator, a cell exhibits an enhanced cycling stability and a good reversibility associated with the Li 2 O 2 formation and decomposition during cell cycling. These results represent a promising progress in the development of an easy-to-operate modified separator for a highly efficient Li-O 2 battery.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Yunxiang Bai,Xinxue Qiu,Deqiang Chen,Junwei Zheng,Liangliang Dong,Chunfang Zhang
Magnetic mixed matrix membranes (MMMs) show great potential for enhancing O 2 /N 2 separation efficiency by leveraging the inherent magnetic property differences between O 2 (paramagnetic) and N 2 (diamagnetic). However, one of the major challenges is the establishment and precise control of magnetic channels between magnetic fillers and polymer matrix. To address this issue, herein, ZIF-8 wrapped Fe 3 O 4 nanoparticles (Fe 3 O 4 @ZIF-8) were synthesized using a step-by-step assembly method, and then integrated into polymer of intrinsic microporosity (PIM-1) matrix to develop MMMs with well-defined magnetic channels for O 2 /N 2 separation. In comparison with Fe 3 O 4 , Fe 3 O 4 @ZIF-8 nanoparticles exhibited significantly enhanced compatibility with the polymer matrix, thereby facilitating uniform dispersion and improving interfacial adhesion. Gas permeation experiments revealed that the magnetic PIM-1/Fe 3 O 4 @ZIF-8 MMMs demonstrated enhanced O 2 /N 2 separation performance due to the combined effects of magnetic responsiveness and the presence of ZIF-8 magnetic channels. Under a magnetic field strength of 56mT, the magnetic MMM with a 4 wt% loading of Fe 3 O 4 @ZIF-8 exhibited optimal O 2 /N 2 separation performance with O 2 permeability of 710 Barrer and O 2 /N 2 selectivity of 3.64. These values represented a significant improvement of 42% and 24%, respectively, compared to pure PIM-1 membrane. Moreover, the simultaneous improvement of permeability and selectivity enabled the achievement of Robeson’s 2008 upper bound for O 2 /N 2 separation, underscoring the great potential of Fe 3 O 4 @ZIF-8 nanoparticles for designing magnetic MMMs with favorable structural attributes and exceptional separation efficiency.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2013
·
IF 3.473
Xiaofeng Xu,Peng Liao,Songhu Yuan,Man Tong,Mingsen Luo,Wenjing Xie
A novel Pd-based electro-Fenton process has recently been developed to degrade organic contaminants in wastewaters and groundwater. However, the high cost of Pd catalyst limits the application of this process. In this study, Cu supported on bamboo charcoal (Cu/C) was synthesized to evaluate the feasibility of substituting Pd catalysts. Using phenol as a probe organic contaminant, the performance of Cu/C catalyst was evaluated for the electro-Fenton degradation of phenol in a typical undivided electrolytic system. The electrochemical degradation of phenol in the presence of Cu/C was significant, following a pseudo-first-order kinetics with rate constant ( k 1 ) of 0.008 min −1 . The addition of Fe 2+ remarkably enhanced the degradation ( k 1 = 0.012 min −1 ). H 2 O 2 and OH were validated as the reactive oxidizing species (ROSs), and OH was the main ROS contributing to phenol degradation. The as-synthesized Cu/C consisting of Cu, CuO and Cu 2 O could catalyze the production of H 2 O 2 from chemisorbed H 2 and O 2 as well as the decomposition of H 2 O 2 to OH. Particularly, the addition of Fe 2+ facilitated the transformation of H 2 O 2 to OH. Phenol degradation increased with increasing the current from 5 to 50 mA and decreased with the further increase to 100 mA. The degradation improved with the increase in Cu loadings and the decrease in solution pH. The presence of NaNO 3 , Na 2 SO 3 or Na 2 S inhibited the degradation, while the presence of NaCl increased the degradation. Although the activity of Cu/C is much lower than that of Pd/C for phenol degradation, the cost of Cu/C is much lower.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Shengqi Ding,Liang Wu,Xianxia Yuan
Electrocatalysts with appropriate electron coupling toward LiO 2 intermediates can exhibit superior oxygen reduction/evolution reaction kinetics in Li-O 2 batteries (LOBs). In this work, a charge redistribution strategy has been developed by constructing NiS/MoS 2 heterostructure nanosheet self-assembled hollow microspheres with an internal electric field to regulate the interaction with LiO 2 and then improve the electrochemical performance of LOBs. Density functional theory calculations and physicochemical characterizations reveal that the difference of work functions between NiS and MoS 2 promotes the electron redistribution in heterointerface via built-in electrical field, leading to increased electron density of interfacial Ni atom, thereby enhancing its electron coupling toward LiO 2 intermediates and promoting one-electron oxygen reduction/oxidation reaction kinetics. As a result, the NiS/MoS 2 -based LOBs exhibit evidently higher discharge capacity and much better cycling performance than the batteries using NiS and MoS 2 . This work provides a reliable charge redistribution strategy induced by build-in electric field to design efficient catalysts for LOBs.
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高影响因子
Small
·
2024
·
IF 13
Qixin Shi,Yingqun Nian,Yang You,Ziyan Li,Yunqi Li,Ran Zhao,Zhengzhi Chen,Tianhang Huang,Bing Hu
Edible bioplastics offer a possible approach with great potential to address the challenges of plastic and microplastic crisis and the issue of food waste. In the present study, in situ, induction of fibrillation of legume proteins within chitosan matrix is found to form edible bioplastic films with a high CO 2 /O 2 selectivity coefficient of ≈130. Desirable mechanical properties, including a high elongation at break of ≈230%, are realized to fabricate shopping bags, which can be filled with 5 kg of fruits. An atmosphere with a high CO 2 content and low O 2 concentration is spontaneously achieved after strawberries are packaged with the films and ≈85% of the fruits are edible after 9 days. The contents of CO 2 in the equilibrium state and the percent of edible fruits are positively correlated with the CO 2 /O 2 selectivity of the films. By comparison of the edible bioplastic films made from mung bean protein (MP) and pea protein (PP), the fibrillation capability of legume proteins and the heterogeneity in polydisperse diameters of the protein fibrils and chitosan are demonstrated to make great contributions to the dense microstructure, leading to the strong mechanical properties and high gas selectivity of the films. The structure-property relationship is elucidated for high-performance bioplastics films.
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高影响因子
MOLECULES
·
2024
·Vol. 29
·期 5
·1094
·
IF 4.2
Hui Liang,Yongxin Zhao,Tongjin Liu,Ruijuan Li,Rumei Li,Yuxiao Zhu,Feng Fang
Zn-doped MnCO3/carbon sphere (Zn-doped MnCO3/CS) composites were synthesized using a simple hydrothermal procedure. Among various samples (ZM-50, ZM-05, and ZMC-0), the ternary Zn-doped MnCO3/CS (ZMC-2) catalyst demonstrated excellent visible light-induced photocatalytic activity. This improvement comes from the Zn addition and the conductive CS, which facilitate electron movement and charge transport. The catalyst exhibited efficient degradation of methylene blue (MB) over a wide pH range, achieving a removal efficiency of 99.6% under visible light. Radical trapping experiments suggested that •OH and •O2−played essential roles in the mechanism of organic pollutant degradation. Moreover, the catalyst maintained good degradation performance after five cycles. This study offers valuable perspectives into the fabrication of carbon-based composites with promising photocatalytic activity.
研究领域:
材料科学
·
环境科学
·
化学
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高影响因子
ENVIRONMENTAL TECHNOLOGY
·
2015
·
IF 1.56
Qunxing Huang,Xu Cai,Moussa Mallaye Alhadj Mallah,Yong Chi,Jianhua Yan
The high concentration of heavy metals in solid wastes may cause serious pollution during thermal treatment. We have investigated, theoretically and experimentally, the effects of several important flue gas species and mineral sorbents on the partitioning behaviour of four major heavy metals (cadmium, lead, zinc and copper) which are often present in municipal solid waste (MSW). Their concentrations in bottom ash, fly ash and flue gas were quantified when model MSW samples were treated thermally under different conditions. The evaporation ratio of the four metals, excluding Cu, increased with decreasing oxygen concentration. The presence of HCl promotes heavy metal evaporation by preventing the formation of stable metallic species, especially for Zn (evaporation of more than 20%). An increase in oxygen concentration has a negative influence on the effect of HCl. In the presence of SO2, Cd and Pb exhibited a higher evaporation ratio, while Zn and Cu were insensitive to the change. SO2 also inhibits Cd vaporization in an oxidative atmosphere. The effect of NH3 on reducing the metal volatilization rate was established indirectly. Calcium oxide addition enhances metal evaporation except for that of Zn (which shows a decrease of 38%). Although desulphurization by calcium injection decreases the volume of acid gas, calcium affects heavy metal pollution control adversely. The presence or addition of SiO2- or Al2O3-containing minerals can lead to the formation of stable metallic salts. This may favour the control of Cd, Pb, Zn and Cu volatilization up to 13%, 50%, 17.5% and 19%, respectively.
研究领域:
环境科学
·
废物处理
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高影响因子
Molecular Catalysis
·
2020
·
IF 3.687
Hai-Min Shen,Lei Liu,Bei Qi,Meng-Yun Hu,Hong-Liang Ye,Yuan-Bin She
Non-solvent and non-additive oxidation of secondary benzylic C–H bonds to aromatic ketones utilizing simple metalloporphyrins as catalysts and O 2 was investigated systematically. Based on systematical studies on reaction parameters, such as the structures of porphyrins, the types of central metals, the amount of catalyst, the pressure of oxygen, and the temperature, most aromatics with secondary benzylic C–H had been converted efficiently and selectively to their corresponding aromatic ketones catalyzed by the optimized metalloporphyrin catalyst T(2,3,6-triCl)PPCo. And the selectivity towards aromatic ketones reached up to 80 %–95 % with acceptable conversions in lower catalyst-loading (2.4 × 10 −3 %, mol/mol). The highest selectivity was achieved for substrate 1,2,3,4-tetrahydronaphthalene with the selectivity of 95.0 % in the conversion of 46.3 %. The superior catalytic performance of T(2,3,6-triCl)PPCo could be mainly ascribed to its excellent plane structure, superior ability for electron transfer and low positive charge around the central metal. All of above properties promoted the formation of catalytic active species high-valence cobalt-oxo complexes, and facilitated the approach of substrates to the catalytic active centers. This work presented an optimized balance among higher selectivity, milder conditions, lower catalyst-loading, and simpler catalysts compared with current documents, which was not only an efficient, practical and significant strategy to functionalize the widely available aromatics possessing secondary benzylic C H with high efficiency and selectivity under milder conditions, but also an important instance in the effective functionalization and utilization of other C H bonds employing optimized catalytic systems based on metalloporphyrins.
研究领域:
有机化学
·
催化化学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Yingying Zhang,Qiang Huang,Ruoting Wang,Xinjie Du,Yu Yu,Zhe Chen
Modulating the coordination environment of single-atom catalysts (SACs) and designing architectures to maximize the exposure of active sites are pivotal strategies for enhancing peroxymonosulfate (PMS) activation. The fabrication of single-atom‑iron catalysts on support with particular coordination is essential but still remains challenge. Herein, we proposed the construction of single-atom‑iron embedded in graphitic carbon nitride nanosheets (SA-Fe@C 3 N 4 ) catalyst. The layer-confined synthesis strategy realized the loading of single-atom irons and ultrathin C 3 N 4 nanosheet formation in the interlayer of layered template RUB-15. XANES analysis corroborated that the isolated iron atoms are coordinated with three nitrogen and one oxygen atoms (Fe-N 3 O 1 ). Notably, the single iron atoms within the SA-Fe@C 3 N 4 matrix serve as the predominant active sites for PMS activation. The catalyst exhibited exceptional activity for the degradation of sulfamethoxazole (SMX), achieving a mass-normalized rate constant ( k Fe ) of 1.54 × 10 5 min −1 mol −1 with high selectivity toward 1 O 2 /•O 2 − .Theoretical calculations revealed that the Fe-N 3 O 1 moiety accelerated the PMS adsorption and reduced energy barriers for the activation of PMS, thus produce key *O intermediate SO 5 •- and form 1 O 2 /•O 2 − with nearly 100% selectivity. This study supplied a simple avenue to fabricate single-atom‑iron on C 3 N 4 with regulated coordination for wastewater treatment.
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