ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Liying Hao,Jikui Sun,Qingyin Wang,Haijiao Xie,Xiangui Yang,Qiang Wei
As an atom-economical reaction, the direct generation of dimethyl carbonate (DMC) and ethylene glycol (EG) via the transesterification of CH3OH and ethylene carbonate (EC) has several promising applications, but the exploration of carriers with high specific surface areas and novel heterogeneous catalysts with more basic sites remains a long-standing research challenge. For this purpose, herein, a nitrogen-doped mesoporous carbon (NMC, 439 m2/g) based K–O2 Lewis base catalyst (K–O2/NMC) with well-dispersed strongly basic sites (2.23 mmol/g, 84.5%) was designed and synthesized. The compositions and structures of NMC and K–O2/NMC were comprehensively investigated via Fourier transform infrared spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy, scanning electron microscopy, transmission electron microscopy, N2 adsorption–desorption, CO2 temperature-programmed desorption, and contact angle measurements. The optimal structural configuration and electron cloud distribution of the K–O2/NMC catalyst were simulated using first-principles calculations. The electron transfer predominantly manifested as a flow from K–O to C–O/C–N, and the interatomic interactions between each atom were enhanced and exhibited a tendency for a more stable state after redistribution. Furthermore, the adsorption energies (Eads) of CH3OH at K–O–O and K–O–N sites were −1.4185 eV and −1.3377 eV, respectively, and the O atom in CH3OH exhibited a stronger adsorption tendency for the K atom at the K–O–O site. Under the optimal conditions, the EC conversion, DMC/EG selectivity, and turnover number/frequency were 80.9%, 98.6%/99.4%, and 40.5/60.8 h–1, respectively, with a reaction rate constant (k) of 0.1005 mol/(L·min). Results showed that the heterogeneous K–O2/NMC catalyst prepared herein greatly reduced the reaction cost while guaranteeing the catalytic effect, and the whole system required a lower reaction temperature (65 °C), a shorter reaction time (40 min), and a lower catalyst amount (2.0 wt % of EC). Therefore, K–O2/NMC can be used as a catalyst in different transesterification reactions.
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JOURNAL OF NANOBIOTECHNOLOGY
·
2024
·Vol. 22
·期 1
·1-15
·
IF 10.6
Li Jingchao,Wang Tingting,Shi Yuanfei,Ye Zichen,Zhang Xun,Ming Jiang,Zhang Yafei,Hu Xinyan,Li Yun,Zhang Dongsheng,Xu Qianhe,Yang Jun,Chen Xiaolan,Liu Nian,Su Xinhui
Radionuclides internal radiotherapy (RIT) is a clinically powerful method for cancer treatment, but still poses unsatisfactory therapeutic outcomes due to the hypoxic characteristic of tumor microenvironment (TME). Catalase (CAT) or CAT-like nanomaterials can be used to enzymatically decompose TME endogenous H 2 O 2 to boost TME oxygenation and thus alleviate the hypoxic level within tumors, but their effectiveness is still hindered by the short-lasting of hypoxia relief owing to their poor stability or degradability, thereby failing to match the long therapeutic duration of RIT. Herein, we proposed an innovative strategy of using facet-dependent CAT-like Pd-based two-dimensional (2D) nanoplatforms to continuously enhance RIT. Specifically, rationally designed 2D Pd@Au nanosheets (NSs) enable consistent enzymatic conversion of endogenous H 2 O 2 into O 2 to overcome hypoxia-induced RIT resistance. Furthermore, partially coated Au layer afford NIR-II responsiveness and moderate photothermal treatment that augmenting their enzymatic functionality. This approach with dual-effect paves the way for reshaping TME and consequently facilitating the brachytherapy ablation of cancer. Our work offers a significant advancement in the integration of catalytic nanomedicine and nuclear medicine, with the overarching goal of amplifying the clinical benefits of RIT-treated patients. Graphical abstract
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Advanced Healthcare Materials
·
2024
·
IF 10
Ming-Xuan Liu,Yan-Chao Liu,Yu-Ting Cai,Ying-Ying Gu,Ya-Qi Zhu,Nan Zhang,Wei-Zhong Zhu,Yong-Hong Liu,Lei Yu,Qi-Tao Zhang,Xiao-Ling Zhang
Hypoxia can aggravate tumor occurrence, development, invasion, and metastasis, and greatly inhibit the photodynamic therapy (PDT) effect. Herein, carbon nitride (CNs)-based DNA and photosensitizer co-delivery systems (BPSCNs) with oxygen-producing functions are developed to address this problem. Selenide glucose (Seglu) is used as the dopant to prepare red/NIR-active CNs (SegluCNs). The tumor-targeting unit Bio-PEG 2000 is utilized to construct BPSCNs nanoparticles through esterification reactions. Furthermore, DNA hydrophobization is realized via mixing P53 gene with a positively charged mitochondrial-targeted near-infrared (NIR) emitting photosensitizer (MTTPY), which is encapsulated in non-cationic BPSCNs for synergistic delivery. Ester bonds in BPSCNs@MTTPY-P53 complexes can be disrupted by lipase in the liver to facilitate P53 release, upregulated P53 expression, and promoted HIF-1α degradation in mitochondria. In addition, the oxygen produced by the complexes improved the hypoxic microenvironment of hepatocellular carcinoma (HCC), synergistically downregulated HIF-1α expression in mitochondria, promoted mitochondrial-derived ferroptosis and enhanced the PDT effect of the MTTPY unit. Both in vivo and in vitro experiments indicated that the transfected P53-DNA, produced O 2 and ROS by these complexes synergistically led to mitochondrial-derived ferroptosis in hepatoma cells through the HIF-1α/SLC7A11 pathway, and completely avoiding PDT resistance caused by hypoxia, exerting a significant therapeutic role in HCC treatment.
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Catalysis Science & Technology
·
2020
·Vol. 10
·期 21
·7378-7385
·
IF 5.721
Mengna Ding,Fengyan Shi,Huijuan Zhu,Yuping Yang,Jiahui Zhong,Liulin Luo,Yuning Huo,Hexing Li
A hybrid Cu2O/TiO2 composite loaded on a Cu mesh (Cu2O/TiO2@Cu mesh) was developed via a supercritical solvothermal route. A uniformly distributed Cu2O/TiO2 p–n hetero-junction was stably coated on a Cu mesh, benefiting the visible-light harvesting. In comparison to electrochemistry and visible-light photocatalysis, the photoelectrochemistry process on the photoanode of the Cu2O/TiO2@Cu mesh presented improved bacterial inactivation activity for Acinetobacter baumannii. By means of the main active species of ˙O2− radicals, the photoelectrocatalytic process on the Cu2O/TiO2@Cu mesh also realized complete leakage of K+ ions, much stronger mineralization of the cell membrane and more efficient elimination of the self-recovery function, finally leading to cell death. In comparison, the electrochemistry process only led to the leakage of K+ ions without inactivation of bacteria, and the visible-light photocatalysis process induced partial leakage of K+ ions and cell mineralization after the death of most bacteria.
研究领域:
环境科学
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材料科学
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微生物学
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光电催化
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CATALYSIS LETTERS
·
2025
·Vol. 155
·期 9
·1-16
·
IF 2.4
Hu Rui,Wang Haiyin,Luo Jiahui,Song Jianjun,Jia Haiyuan
Peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs) have been proven to be an effective method for the removal of tetracycline in water. In this study, the Co 3 O 4 /molecular sieve catalyst synthesized by the incipient wetness impregnation method was used for PMS activation. The effect of specific surface area on the catalytic performance of Co 3 O 4 /molecular sieve catalyst was investigated and analyzed in detail by characterization techniques. In the Tetracycline hydrochloride (TCH) degradation experiment, the Co 3 O 4 /13X catalyst exhibited the highest specific surface area (490.584 m 2 /g) and provide abundant active sites, enabling 98.0% TCH degradation within 30 min under optimal conditions (1.5 g catalyst, 0.3 mM PMS, pH 8.0, 25℃), with a reaction rate constant (k obs ) of 0.0977 min -1 . In addition, the degradation mechanism of TCH was explored using electron paramagnetic resonance (EPR) spectroscopy and quenching experiments. It was confirmed that free radicals (SO 4 •− , •OH, O 2 •− ) and non-free radical species ( 1 O 2 ) generated during the reaction play a crucial role in the degradation process of TCH. In summary, the Co 3 O 4 /13X catalyst, when activating PMS, exhibits a remarkable synergistic effect on the degradation of TCH, and shows good repeatability and environmental adaptability. This study provides valuable insights into the design and optimization of catalysts for degrading antibiotic pollutants in water treatment processes. Graphical
研究领域:
环境科学
·
催化
·
水处理
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化学工程
·
污染物降解
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Nano Energy
·
2024
·
IF 16.8
Zuheng Jin,Xiao Zheng,Zhihong Zhu,Chuan Jiang,Sha Wu,Changzheng Hu,Laijun Liu,Liang Fang,Zhenxiang Cheng
Considering advanced oxidation techniques offer new opportunities for microbial degradation and inactivation, in this study, Z-type heterojunctions of Ba 1.4 Sr 3.6 NdNb 7 Ti 3 O 30 -N 2 /g-C 3 N 4 (BN 2 /CN) were successfully prepared using a solid-phase method and explored for their potential applications in tribocatalytic bactericidal inhibition. These results demonstrate that BN 2 /CN exhibits excellent inhibitory and inactivating effects on E. coli under tribocatalytic conditions. The UV–visible spectrum showed a gradual decrease in the survival rate of E. coli with the increase of tribocatalysis time, reaching an inactivation effect of 91% after 1 h, while fluorescence staining also confirmed that E. coli were essentially eliminated, with hardly any surviving bacteria observed under a laser confocal microscope . Hence, this study presents a novel catalytic approach for sterilization. Moreover, inhibition experiments demonstrated that the BN 2 /CN catalyst did not inhibit the growth of E. coli, tribocatalysis played a crucial role in the disinfection and sterilization processes . The inactivation of bacteria by BN 2 /CN catalyst was still above 90% after multiple cycles of sterilization experiments. Finally, we demonstrated that the production of •OH and •O 2 - during tribocatalysis is key to the inactivation of E. coli, thus achieving the desired effect of tribocatalytic sterilization.
研究领域:
催化
·
材料科学
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微生物学
·
环境科学
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COMPOSITES PART B-ENGINEERING
·
2021
·
IF 9.078
Yang Zhan,Shao-hua Luo,Jian Feng,Lin Zhang,Xin Liu,Qing Wang,Ya-hui Zhang
The lithium-oxygen batteries (LOBs) have gained extensive interest in the past decade, but are plagued by slow reaction kinetics and induced large-voltage hysteresis. Therefore, developing extremely capable catalysts to enhance catalytic behavior and mitigate oxidation-reduction overpotential of LOBs is of huge challenge and significance. Attributable to their economically friendly and great activity, transition metal oxides (TMO) have incurred lots of attention as alternative electrocatalysts to replace the currently used noble metal-based catalysts. In this work, we fabricate a highly efficient TMO (the MIL-88A heated at 500 °C under protective flow, M8-Fe 3 O 4 @NC-500) electrocatalyst as advanced cathodes, which attributed to its unique structure, numerous dendritic-shaped carbon layer was anchored inplane into the micrometer-long spindle-shaped prisms with evenly distribution and contains abundant Fe–N/Graphitic N active sites. Therefore, the LOBs (based on M8-Fe 3 O 4 @NC-500/AB cathode) deliver superior electrochemical performance with large specific capacities of 14866.1 mAh g −1 , low overpotentials (1.31 V), and steady cycling stability (553 cycles, limited 500 mAh g −1 , under 0.05 mA cm −2 ). Our work provides a novel vision to rationally design and synthesize a powerful TMO electrocatalyst (with the 2D carbon nanosheet coating) for the LOBs cathode.
研究领域:
材料科学
·
电化学
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MOLECULAR PHARMACEUTICS
·
2025
·
IF 4.5
Xin Yue,Qian Lin,Xiaohang Liu,Zhaoyi Yu,Jiafeng Xu,Xuan Zhu,Jinyan Lin,Aijie Liu
The high intracellular glutathione (GSH) level, naturally hypoxic conditions within the tumor microenvironment, and limited reactive oxygen species (ROS) generation pose significant obstacles to the effectiveness of sonodynamic therapy (SDT). Overcoming these barriers through depletion of GSH and relieving hypoxia offer a promising strategy to enhance SDT effectiveness. Herein, we developed a dendritic tetra-sulfide-bridged mesoporous silica (DTSMO) that encapsulated both chlorin e6 (Ce6) and cerium via channel-limited in situ coordination and is subsequently cloaked with the macrophage cell membrane (MCM) to facilitate efficient reactive oxygen species (ROS)-based therapy via multispecies enzymatic activities. First, this nanosystem exhibited Ce(IV) ions to mimic catalase (CAT)-like activity, converting H2O2 into O2, thereby effectively alleviating tumor hypoxia. Meanwhile, the nanosystem possessed Ce (III)-based peroxidase (POD)-like activity, enabling the conversion of H2O2 into hydroxyl radicals (•OH) while simultaneously depleting GSH. Both in vitro and in vivo experiments demonstrated that GSH depletion exerted a powerful supplementary effect on CDT and SDT, achieving a tumor inhibition rate of up to 96%, without affecting normal tissues during treatment.
研究领域:
纳米医学
·
癌症治疗
·
活性氧
·
酶模拟
·
生物材料
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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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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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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2026
·
IF 12.2
Chunyan Zhang,Jiarong Liu,Qing Cao,Tianzeng Chen,Yonghong Wang,Peng Zhang,Hao Li,Biwu Chu,Xiuhui Zhang,Qingxin Ma,Hong He
The coupled chemical transformation of NOx and SO2 plays a pivotal role in the atmospheric sulfur and nitrogen cycles. While these pollutants show negligible gas-phase interrelationship, they exhibit strong synergistic interactions in multiphase aerosol chemistry, yet their underlying reaction mechanisms remain elusive. We demonstrate that O2 serves as the key mediator enabling efficient coupling between aqueous-phase bisulfite (S(IV)) and nitrite (N(III)) through a previously overlooked reaction pathway at environmentally relevant pH (3.0–6.0). Under isolated conditions at pH 4.4, S(IV) undergoes sluggish O2-driven oxidation (4% sulfate yield), whereas N(III) remains oxidation-resistant. In the absence of O2, S(IV)-N(III) redox reactions yield limited sulfate (4%) and N2O, which is consistent with traditional mechanism cognition. Strikingly, the presence of O2 dramatically enhances co-oxidation, simultaneously producing sulfate (43%) and nitrate (36%). Theoretical calculations identify •HSO3 radicals (from HSO3‐/O2 interaction) as key intermediates that combine with O2/NO2‐ to form transient complexes ([•SO5···ONOH]− and [SO3-NO2···•HO2]−), which ultimately decompose into sulfate and nitrate. Observations in Beijing highlight the dominant role of the S(IV)-N(III) synergistic oxidation mechanism in sulfate formation, surpassing the conventional NO2- and O3-driven pathways. This breakthrough enhances our knowledge of atmospheric chemistry, particularly in the coupled cycling of sulfur and nitrogen, including sulfate/nitrate generation and HONO removal dynamics.
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ELECTROCHIMICA ACTA
·
2026
·
IF 5.8
Jinxin Xie,Yujue Wang,Haisong Li,Yinqiao Zhang,Minghua Zhou
The mass transfer of O 2 /O 3 was improved at three-phase interface of CB‑PTFE. • CB enabled the synergistic reduction of O 2 /O 3 for •OH generation. • O 3 reduction and catalytic ozonation accelerated phenol mineralization. • Phenol removal and mineralization were 100% and 85% in ten-cycles. The electro-peroxone (E-peroxone) process suffered from the limited mass transfer and insufficient utilization of gaseous O 2 /O 3 mixture. Herein, a hydrophobic carbon black‑polytetrafluoroethylene (CB‑PTFE) electrode was fabricated to construct a gas‑liquid‑solid three-phase interface for improving phenol mineralization. The CB-PTFE electrode exhibited a high contact angle of 143.3°, which enhanced the mass transfer of O 2 /O 3 effectively. Compared with the hydrophilic carbon black‑polyvinylidene fluoride (CB‑PVDF) cathode (72.9°, 51.8%), CB‑PTFE achieved 86.0% TOC removal (0.016 min −1 ) at 120 min in E-peroxone, significantly outperforming sole ozonation (O 3 , 40.0%, 0.004 min −1 ) and electro‑oxidation (EO, 7.2%, 0.004 min −1 ). The greater TOC removal in CB-PTFE/O 3 (66.3%, 0.0095 min −1 ) than that in O 3 indicated that CB-PTFE had catalytic ozonation activity. Electrochemical analysis by a rotating ring‑disk electrode (RRDE) revealed that CB enabled simultaneous 2‑electron oxygen reduction reaction (ORR) to H 2 O 2 (n = 2.23) and efficient 1‑electron O 3 electro‑reduction for increased cathodic current and hydroxyl radical (•OH) generation under the O 2 /O 3 atmosphere. The highest •OH yield (280.5 μmol/L) was obtained using hydrophobic CB-PTFE in E‑peroxone, and theoptimal conditions were the applied current of 20 mA, in‑gas O 3 concentration of 50 mg/L and neutral pH of 7.0. Furthermore, the hydrophobic CB‑PTFE electrode maintained nearly 86.0% TOC removal over ten-cycles with stable structural integrity, despite a slight decrease of hydrophobicity. The reduction of O 2 /O 3 , catalytic ozonation and peroxone reaction were coupled in E-peroxone synergistically, which offered a promising strategy for efficient pollutant abatement. Download: Download high-res image (262KB) Download: Download full-size image
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