APPLIED CATALYSIS A-GENERAL
·
2021
·
IF 5.706
Lei Chen,Wenxia Zhuang,Jingmin Lan,Xiaoling Liu,Shi Jiang,Lei Wang,Yu Zhou,Jun Wang
Mg-bearing MTW silicalite zeolite, MgSi-ZSM-12, was straightforwardly synthesized by involving an unusual acidic pre-gelation system and engaged as the task-specific support for loading the Au nanoparticles (NPs). The resulting Au/MgSi-ZSM-12 catalyst showed stably excellent activity for the oxidation of HMF into FDCA in the presence of atmospheric dioxygen (O 2 ) without externally adding any liquid base, affording a yield of 87 % and turnover number (TON) of 331 based on the surface Au sites. Superior basicity was evidenced by embedding Mg species into the all-silica zeolitic skeleton, which enables strong, weak, and near-zero affinity towards aldehyde, alcohol, and carboxyl groups, respectively, thus, allows rapid and high-uptake adsorption of HMF, but negligible adsorption of FDCA. This unique feature of the Mg-bearing all-silica zeolite support together with its synergy with the active sites of Au NPs is revealed to accelerate the production of FDCA under the base-free mild condition.
研究领域:
催化化学
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材料科学
·
环境化学
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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
·
2024
·
IF 5.8
Bei Ren,Ziqian Meng,Bixian Zhang,Sihao Jian,Chufei Cheng,Jiadong Hou,Ruixin Hao,Bo Li,Yang Miao,Chao Ma,Weihua Ji
High-entropy fluorite oxide ceramics are promising candidates for spacecraft applications due to their excellent high-temperature thermal-mechanical properties. In this work, four kinds of high-entropy fluorite oxide ceramics ((ZrHfCeYEr) (1-x)/5 Ti x )O 2-δ (HEFOs, x = 0, 0.025, 0.05, 0.075) with different Ti 4+ contents were successfully synthesized through solid-state reaction method with conventional sintering. They all exhibited phase stability when annealed at 1500 ℃ for 20 h. When the content of Ti 4+ was increased to x = 0.075, the thermal conductivity reduced to1.34 W·m −1 ·K −1 at 1100 ℃, and the hardness and elastic modulus increased to 14.01 GPa and 205.70 GPa, respectively. Furthermore, the cyclic thermal shock resistance of HEFOs at different temperatures was investigated. The initial flexural strength reached 219.03 MPa when the content of Ti 4+ was increased to x = 0.075. After 60 thermal shock cycles at 1200 ℃ and 1500 ℃, the residual strength ratios were 97.56 % and 83.36 %, respectively. The results of this study establish the foundation for future applications of high-entropy fluorite oxide ceramics in spacecraft hot-end components.
研究领域:
材料科学
·
航天工程
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Chen Wang,Yunpeng Zou,Xiaohui Wu,Xiangling Zhang,Wenjiao Sang,Tao Zhou,Mingjie Huang
Realizing efficiently sustainable generation of singlet oxygen ( 1 O 2 ) in the O 2 activation-based systems is crucial, since 1 O 2 can oxidize many organic pollutants via a non-radical pathway that is preferable in complex water matrices e.g. saline wastewaters. In this study, a boosted strategy that introduced oxygen vacancies (OVs) and surface carboxyl groups (−COOH) onto electron-rich copper‑iron oxides, was proposed by a facile mechanochemical ball-milling process with citrate ligands (Cit). Notably, the resulting Cit@CuFe 2.5 O x catalyst enabled efficient O 2 activation via a selective non-radical pathway, achieving a standardized pseudo-first-order rate constant ( k obs ) of 0.073 min −1 ·g −1 for sulfamethoxazole (SMX) degradation, with over 90 % of the oxidative contribution attributed to 1 O 2 . The ball-milling procedure with Cit could cause the generation of abundant OVs for O 2 adsorption and activation . Mechanistic analysis and theoretical calculations revealed that the OVs accelerated electron transfer from adjacent Cu(I) atoms to adsorbed O 2, facilitating the generation of O 2 − and markedly lowering the free energy barrier for its subsequent conversion to 1 O 2 other than H 2 O 2 . Additionally, the surface-bound −COOH groups facilitated the transformation of molecular O 2 to adsorbed O 2 at OVs sites, further lowering the thermodynamic barrier of the O 2 ⟶ O 2 − ⟶ 1 O 2 pathway. This study provides a simple and cost-effective promotional strategy for O 2 activation by ball-milled electron-rich materials, offering an easily obtained method to induce 1 O 2 -dominated oxidation of recalcitrant organic pollutants in the treatment of high-salinity wastewater.
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TALANTA
·
2026
·
IF 6.7
Chao Lu,Xue Fan,Fengna Xi,Yucheng Zhou
Sensitive and parallel individual detection of multiple tumor biomarkers is critical for early diagnosis and therapeutic monitoring of pancreatic cancer. Herein, a ternary electrochemiluminescence (ECL) system was developed by employing nanochannel-confined cerium dioxide (CeO 2 ) nanozyme as co-reactant enhancers for the luminol-dissolved oxygen (DO) system, enabling parallel individual immunoassays of carcinoembryonic antigen (CEA) and carbohydrate antigen 199 (CA199). Vertically-ordered mesoporous silica film (VMSF) was rapidly grown on an indium tin oxide (ITO) electrode, forming nanochannel array with thickness of 97 nm and diameters of 2.7 nm. CeO 2 nanozyme was synthesized in situ within the VMSF nanochannels via electrochemical deposition. Transmission electron microscopy (TEM), high-angle annular dark-field scanning TEM (HAADF-STEM), and energy-dispersive X-ray spectroscopy (EDX) elemental mapping confirmed CeO 2 nanozyme was confined in nanochannels with high dispersion. CeO 2 nanozyme exhibited peroxidase-like catalytic activity and enhanced the ECL intensity of the luminol-DO system by 13.9-fold under near-neutral conditions through catalysis of both oxygen reduction and luminol oxidation. After derivatization of the VMSF outer surface with epoxy groups, antibodies specific to CEA or CA199 were covalently immobilized to construct two immunorecognition interfaces. Target binding formed antigen-antibody complexes, increasing interfacial resistance and hindering diffusion of the ECL emitters, enabling a signal-off immunoassay mode. The resulting immunosensors displayed wide detection linear ranges from 0.1 pg mL −1 to 100 ng mL −1 for CEA and 0.1 × 10 −3 mU mL −1 to 1.0 × 10 4 mU mL −1 for CA199, with limit of detection (LOD) of 1.3 fg mL −1 and 0.5 × 10 −4 mU mL −1 , respectively. Both immunosensors exhibited good selectivity, reproducibility, and storage stability.
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INTERNATIONAL JOURNAL OF ENERGY RESEARCH
·
2022
·Vol. 46
·期 14
·19357-19367
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IF 4.672
Jiuqing Liu,Feifei Song,Junying He,Zikun Hong,Qihou Li,Ya Chen,Lishun Bai,Fanli Zeng,Chen Cheng,Zehao Chen
Summary Owing to its unparalleled theoretical energy density, the Li-O 2 batteries are thought to be one of the most promising energy storage systems, but its application is seriously hindered by its potential safety risks arising from the passivation and corrosion of lithium anode. To address these issues, it is an efficient way to develop functionalized separator that could prevent the migration of anions and macromolecules from cathode toward anode. Herein, a novel Nafion-functionalized polyethersulfone (PES)-based ion-permselective separator was prepared by using non-solvent induced phase separation (NIPS) method. The Nafion ensures a better physical strength of the composite separator, and further characterizations show that the obtained composite separator owns good ionic conductivity (0.52 mS cm −1 ), high lithium ion migration number (0.80), and better cyclic stability (120 cycles, 1000 mAh g −1 ). Consequently, the composite separator serves as an excellent candidate to solve the “shuttle effect” of redox mediators (RMs), the assembled Li-O 2 battery with composite separator adding LiI as RMs presents lower charge overpotential and longer cycle stability (170 cycles, 1000 mAh g −1 ).
研究领域:
材料科学
·
电化学
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DOI
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JOURNAL OF POWER SOURCES
·
2020
·
IF 8.247
Hongying Tang,Kang Geng,Jinkai Hao,Xiaojuan Zhang,Zhigang Shao,Nanwen Li
Quaternized poly(sulfone)s based on trimethylamine (PSf-TMA-x) and triethylamine (PSf-TEA-x) are developed to form quaternary ammonium (QA)-biphosphate ion pairs as promising high temperature proton exchange membrane (HT-PEM) in H 2 /O 2 fuel cells. The strong QA-biphosphate ion-pair interaction results in high acid absorption and thus high proton conductivity of 78.1 mS cm −1 for PSf-TEA-110/PA membrane at 160 °C in spite of its lower degree of functionalization. Thus, the peak power density of more than 400 mW cm −2 is achieved at 160 °C for the quaternized PSf membranes in H 2 /O 2 fuel cell, which is higher than that of the poly(benzeimidazole) ( m -PBI) membrane (370 mW cm −2 ). Subsequently, the degradation mechanism of the PSf membranes is demonstrated using NMR technique to be occurred in both the polymer backbone and the QA groups. The stability investigation of model compounds further confirms that the degradation of the membranes resulted from the scission of ether linkage and isopropylidene group and the SN2 nucleophilic substitution of QA at operating conditions. Therefore, the significant performance decrease is observed and the lifetime is only less than 30 h at 200 mA cm −2 which is much lower than that of m -PBI membrane (>40 h).
研究领域:
材料科学
·
化学工程
·
能源科学
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DOI
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2018
·
IF 4.61
Sharafat Ali,Izaz Ali Shah,Aziz Ahmad,Javed Nawab,Haiou Huang
In this study, pristine multi-walled carbon nanotubes (MWCNTs) were functionalized by using Ar/O 2 plasma treatment technique, which enhanced adsorptive membrane filtration of zinc ions from water and wastewater. The XPS analysis showed that plasma treatment largely increased the surface oxygen groups content of MWCNTs from 2.78% to 6.79%. This change increased the surface negative charged, dispersion and adsorption properties of MWCNTs without causing any damages to the integrity of the nanotube pattern. Pressure-driven filtration of plasma-treated MWCNT (P-CNT) dispersion formed a stable layer inside the lumen of a hollow fiber membrane. The contact angle analysis demonstrated that after incorporation of P-CNT into the HF membrane increased membrane hydrophilicity. The P-CNT membrane effectively removed almost 100% of zinc from synthetic waters and approximately 80% of zinc from a wastewater effluent by surface complexation reaction. A follow-up regeneration study demonstrated that the adsorptive removal of zinc by the CNT membrane was reversible under selected conditions, thus making it possible to repeatedly use the membrane for long-term zinc filtration. This study suggests that HF membranes modified with P-CNTs possess superb adsorption properties for metal ions , allowing the operation of CNT membranes for water treatment .
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JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Xiaohong Zou,Qian Lu,Cuie Wang,Sixuan She,Kaiming Liao,Ran Ran,Wei Zhou,Liang An,Zongping Shao
Before the practical application of the Li–O 2 battery (LOB), a critical issue regarding large overpotential upon charging (which causes irreversible side reactions and low energy efficiency) should be resolved. The utilization of redox mediators (RMs) which oxidatively decompose insulating discharge product, Li 2 O 2 , is one promising solution to address this issue. However, the soluble RMs can easily diffuse to and react with the Li metal anode (encountering Li dendrites is even worse). Here, a chemical self-assembly strategy is introduced into the fabrication of the iodide-redox-phobic and Li-ion-philic membrane for LOBs, in which the electronegative δ-MnO 2 layer is in-situ grown on commercial polyethylene (PE) membrane (MnO 2 @PE). The electronegative MnO 2 layer can simultaneously repel the shuttle of iodide species and regulate the uniform Li + deposition. Controlling cut-off capacity of 1000 mAh g −1 , iodide-redox-based LOB with MnO 2 @PE demonstrates low overpotentials (∼0.7 V vs. Li + /Li), dendrite-suppressing capability, as well as impressive long-term reversibility over 500 cycles (2000 h), which urges the LOB technology competitive among the next-generation rechargeable power systems.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Junjie Wu,Peng Shen,Xian Qin,Yulu Yang,Chuanchuan Lin,Xuan Li,Wenbo Geng,Pengfei Gao,Lixue Chen,Li Miao,Yang Jiao,Bailong Tao
Bacterial wound infection is a major challenge to human health worldwide. In this study, a composite nanogenerator, CaO 2 @ZIF-67-PLL, was fabricated via a bottom-up approach with chemodynamic therapy (CDT)/hypoxia improvement for rapid therapy of biofilm-infected wounds. Under a pathologically acidic microenvironment, the out layer ZIF-67 can be decomposed to rapidly release Co 2+ and CaO 2 ; Subsequently, the unprotected CaO 2 reacts with H 2 O to produce O 2 and H 2 O 2 . The self-supply of O 2 relieves hypoxia and inflammatory response induced by infections, while the generated H 2 O 2 and poly- l -lysine (PLL) exhibited synergistic strong anti-biofilm capability against Escherichia coli ( E. coli) and Staphylococcus aureus (S. aureus) as assessed by reactive oxygen species (ROS) generation, membrane permeability change, ATP reduction, o -nitrophenyl-β-d-galactopyranoside (ONPG) hydrolysis and intracellular component leakage. Meanwhile, CaO 2 @ZIF-67-PLL exhibited good cytocompatibility and promoted the adhesion, proliferation, and migration of NIH-3T3 cells by enhancing the expression of wound healing-related genes (TGF-β1, VEGF, α-SMA, Col I, Col III, and Wnt-5a). Notably, CaO 2 @ZIF-67-PLL could significantly improve the healing process of S. aureus -infected wounds via suppressed inflammatory responses, enhanced collagen disposition and angiogenesis, and stimulated HIF-1α, CD31, and Wnt-5a/β-Catenin signaling pathways. These results indicated the potential of CaO 2 @ZIF-67-PLL nanogenerator for clinical application in infected wound treatment.
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Advanced Healthcare Materials
·
2023
·Vol. 12
·期 15
·2202280
·
IF 10
Wenya Li,Rongtian Li,Qiang Ye,Yiming Zou,Xing Lu,Wenhua Zhang,Jinxiang Chen,Yinghua Zhao
Nanomedicine exhibits emerging potentials to deliver advanced therapeutic strategies in the fight against triple-negative breast cancer (TNBC). Nevertheless, it is still difficult to develop a precise codelivery system that integrates highly effective photosensitizers, low toxicity, and hydrophobicity. In this study, PCN-224 is selected as the carrier to enable effective cancer therapy through light-activated reactive oxygen species (ROS) formation, and the PCN-224@Mn 3 O 4 @HA is created in a simple one-step process by coating Mn 3 O 4 nanoshells on the PCN-224 template, which can then be used as an “ROS activator” to exert catalase- and glutathione peroxidase-like activities to alleviate tumor hypoxia while reducing tumor reducibility, leading to improved photodynamic therapeutic (PDT) effect of PCN-224. Meanwhile, Mn 2+ produced cytotoxic hydroxyl radicals (∙OH) via the Fenton-like reaction, thus producing a promising spontaneous chemodynamic therapeutic (CDT) effect. Importantly, by remodeling the tumor microenvironment (TME), Mn 3 O 4 nanoshells downregulated hypoxia-inducible factor 1 α expression, inhibiting tumor growth and preventing tumor revival. Thus, the developed nanoshells, via light-controlled ROS formation and multimodality imaging abilities, can effectively inhibit tumor proliferation through synergistic PDT/CDT, and prevent tumor resurgence by remodeling TME.
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ELECTROCHIMICA ACTA
·
2022
·
IF 7.336
Jie Li,Youcai Lu,Shiyu Ma,Zhongjun Li,Qingchao Liu
Li–O 2 battery has attracted wide attention because it can satisfy the need for a new energy storage system with high energy density. However, poor oxygen reduction (ORR)/oxygen evolution (OER) kinetics involving Li 2 O 2 formation/decomposition is a major obstacle to its development. By designing suitable cathode with desired structure and surface electronic states, the formation/morphology of Li 2 O 2 and the reaction kinetics of charge process can be efficiently optimized simultaneously. In this work, a novel sulfur (S) and chlorine (Cl) co-doped porous carbon (CSC) were synthesized by one-step pyrolysis strategy, and the amount of heterogeneous atoms could be flexibly controlled by different calcination temperatures . Experimental combined with theoretical calculations show that the content of C Cl bond plays an important role in the adsorption of intermediate LiO 2 , thus regulating the morphology of Li 2 O 2 and ultimately affecting the release of battery energy. The C S bond mainly acts on the dynamics of the ORR and OER processes, which has an important influence on improving the round-trip efficiency of the battery. Benefiting from the synergistic effect of heteroatoms , the electrochemical performances of the Li–O 2 battery, including round-trip efficiency, discharge capacity and cycling stability are greatly improved.
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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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