RESEARCH ON CHEMICAL INTERMEDIATES
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2025
·
IF 3.5
Yan Jiaqi,Chen Wenkai,Ni Wenjin,Li Lu,Fu Jinfeng,Yang Qian,Yang Zhiyong
N -cyclohexylcyclohexanimine (N-CCA), a by-product of cyclohexylamine (CHA) oxidation to cyclohexanone oxime (CHO), was used as the starting reactant for the efficient conversion to CHO under an oxygen atmosphere, utilizing the constructed surface hydroxyl-rich Ti-based catalysts. Of these, the 20% TiO 2 /Hβ catalyst exhibited unique catalytic activity and stability, achieving 45.9% N-CCA conversion and 82.1% CHO selectivity, with the content of high-boiling by-products not exceeding 1.0%. The superior catalytic performance, as evidenced by characterization results, stems primarily from: (i) the combination of TiO 2 and Hβ, which promotes the formation of a high specific surface area with fine TiO 2 nanoparticles and high-density Ti δ+ active sites, which facilitate the adsorption and activation of N-CCA; (ii) the construction of rich hydroxyl groups, which enhances the Brønsted acid sites, thereby improving the generation of active oxygen species; (iii) the intercrystalline embedding of TiO 2 and Hβ, which forms Ti–O–Si bonds, effectively inhibiting Ti leaching and ensuring excellent catalyst stability. The conversion of N-CCA, the main by-product of CHA oxidation, to the desired CHO using an efficient and robust 20% TiO 2 /Hβ catalyst represents an attractive pathway.
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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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PubMed
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Inorganic Chemistry Frontiers
·
2025
·
IF 6.4
Kexin Yang,Zhijia Song,XiaoXiao Fu,Wei Yan,Tao Zhang,Yiwei Hua,Haixin Lin,Qin Kuang,Zhaoxiong Xie
The photocatalytic direct one-step two-electron (2e-) oxygen reduction reaction (ORR) holds great potential in efficient H2O2 synthesis. However, it is still a significant challenge to design photocatalysts for achieving high-efficiency H2O2 production via this direct one-step 2e- ORR pathway. To address this, we have constructed a Z-scheme BAIO/C3N4 heterojunction by in situ growing Ba2AgIO6 (BAIO) on the surface of C3N4 nanosheets. Under visible light irradiation, the optimal sample, with a BAIO:C3N4 mass ratio of 1:1.5, exhibited a remarkable H2O2 yield of up to 535.9 μmol g-1 h-1, which is 8.8 times higher than that of pure C3N4. This enhancement is attributed to the improved charge separation and migration efficiency facilitated by the enhanced internal electric field (IEF) in BAIO/C3N4 heterojunction. Furthermore, the heterojunction altered the O2 adsorption configuration to the Yeager-type, promoting a more efficient and selective direct one-step 2e- ORR for H2O2 production. This study highlights the importance of regulating the reaction pathway to enhance photocatalytic H2O2 production activity and offers a new insight for designing highly active photocatalysts.
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GREEN CHEMISTRY
·
2025
·
IF 9.2
Yongji Xia,Sheng Lin,Jian Yan,Renjie Xu,Yingpeng Du,Chunxiao Song,Dong-Liang Peng,Zhidong Zhou,Jiajia Han,Guanghui Yue
Spinel-type Co3O4 has been identified as a highly prospective cathode catalyst for lithium-oxygen batteries (LOBs), attributable to its distinctive bimetallic active sites that manifest exceptional bifunctional catalytic characteristics. Nonetheless, the practical implementation of this process is constrained by the inherent conductivity limitations of Co3O4 and the suboptimal utilization of active sites. In this study, a Cu-Mn bimetallic doping strategy is employed to prepare a spherical-like structure of Co3O4 formed by self-assembling one-dimensional nanorods. The introduction of Cu²⁺ results in a reduction of the surface energy of the system, thereby facilitating the directional growth of the nanorods. The redox-active Mn³⁺/Mn⁴⁺ pairs exhibit an inhibitory effect on Ostwald ripening, achieved by stabilizing the fine particles during synthesis and regulating solute diffusion kinetics. This combined action of Cu and Mn enhances active site exposure and optimizes charge transfer kinetics. Furthermore, the doping of bimetallic ions resulted in the redistribution of the Co3+/Co2+ ratio, optimizing the electronic structure for efficient charge transfer during the reaction. The combination of tailored electronic states and optimized nanostructures demonstrates excellent dual-functional catalytic activity for ORR and OER, with a half-wave potential of 0.71 V (vs RHE) for OER and an overpotential of 400 mV (10 mA cm-2) for ORR. The assembled LOBs can be stably cycled up to 450 cycles and an ultra-high discharge capacity of 7268 mAh g-1 for LOBs. This study provides a novel reference for the design of efficient bifunctional catalysts.
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Catalysts
·
2025
·Vol. 15
·期 5
·459
·
IF 4
Dan Wang,Yanan Liu,Kun Wan,Danning Feng,Yan Pei,Minghua Qiao,Xiaoxin Zhang,Baoning Zong
The electrocatalytic reduction of O2via two-electron reaction (2e-ORR) to H2O2represents a promising alternative to the current anthraquinone process, since it is advantageous in the sustainable and decentralized production of H2O2. Herein, we report the development of oxygen and nitrogen-rich few-layered graphene-like materials (ms-dcda) by the one-step carbonization of biomass-sourced monosaccharides (D-glucose, D-fructose, D-galactose, D-ribose, D-xylose, L-arabinose, and D-mannose) with the aid of dicyandiamide for electrochemical O2reduction to H2O2. The ms-dcdamaterials were porous and possessed wrinkled morphology typical of graphene nanosheets. In H2O2production via 2e-ORR in an acidic electrolyte, these ms-dcdamaterials were all active and stable catalysts, among which glu-dcdaderived from D-glucose and dicyandiamide displayed the lowest onset potential of 0.553 V and the highest selectivity of up to 91.6%. The catalyst was also highly stable in chronoamperometric tests. Selective chemical titration of the C–OH and C=O groups revealed that the latter is far more active and selective than the former in 2e-ORR. Moreover, a positive correlation between the contents of C=O and pyrrolic N and the H2O2partial current suggests that the pyrrolic N group also contributes to 2e-ORR. This work affords a facile strategy for the sustainable fabrication of metal-free carbon-based catalysts efficient for H2O2electrosynthesis.
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NEW CARBON MATERIALS
·
2025
·
IF 6.8
Xiu-zhen LV,Xiang-xiang XU,Meng-meng YU,Yi-chen WEI,Jun-ying WANG,Jun-zhong WANG
The need for bi-functional catalysts that facilitate both the oxygen reduction (ORR) and carbon dioxide reduction (CO 2 RR) reactions arises from their potential to help solve the critical problems of carbon neutrality and renewable energy conversion. However, there are few reports on the development of bi-functional catalysts for zinc-air battery-driven CO 2 RR devices. We introduce a novel approach for synthesizing Fe 2 N/Fe 3 C species embedded in nitrogen-doped carbon nanofibers by electrospinning a solution of Hemin and polyacrylonitrile in N,N-dimethylformamide. The material has an exceptional catalytic performance, with a half-wave potential of 0.91 V versus RHE for the ORR and values of over 90% for both the selectivity and Faradaic efficiency for the CO 2 RR. The high catalytic performances are attributed to the strong coupling between the Fe 3 C/Fe 2 N heterostructure and the Fe-N-C sites in the nitrogen-doped carbon nanofibers. Notably, both Fe 3 C and Fe 2 N play distinct roles in both the ORR and CO 2 RR. This investigation indicates a way for designing advanced carbon-based bi-functional catalysts for use in this field.
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Catalysts
·
2025
·Vol. 15
·期 6
·545
·
IF 4
Xiaohong Yao,Jian Zhang,Chao Long
This study explored how pore size engineering in Nb-Mn/MCM-41 catalysts affects plasma-catalytic toluene oxidation. Adjusting the pore diameter (2.49–3.98 nm) modulated metal-support interactions and oxygen dynamics, with pore expansion to 3.73 nm (M3) optimizing the Mn4+/(Mn2++ Mn3+) ratio (XPS: 36.8%), the amount of lattice oxygen species (O2-TPD: 0.222 mmol/g), and crystallite size control (1.5 ± 0.2 nm, TEM). Smaller pores (M1: 2.49 nm) enhanced toluene adsorption but limited active site accessibility, while oversized pores (M4: 3.98 nm) reduced oxygen storage capacity (0.600→0.412 mmol/g). The Nb-Mn/M3 catalyst achieved superior performance with 96.8% toluene conversion, 55.0% CO2selectivity, and 85.4% carbon balance, while minimizing organic byproducts (GC-MS). Mechanistic studies revealed pore-mediated oxygen storage-transport cycles as critical for decoupling adsorption and oxidation steps. This study reveals fundamental mechanisms linking pore architecture to plasma-catalytic synergy in toluene oxidation, offering critical insights for the systematic design of energy-efficient, plasma-catalytic systems targeting industrial VOCs remediation.
研究领域:
催化化学
·
环境化学
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材料科学
·
等离子体化学
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纳米技术
·
表面科学
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Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 8
·4880-4889
·
IF 12.732
Wei Wu,Wang Lin,Hongjiang Chen,Keyan Wei,Zhitong Li,Haitao Yang,Mingxian Liu,Huaicheng Xiang,Libo Deng,Lei Yao
The development of high-performance solid-state batteries (SSBs) that integrate high safety with high energy density has long been pursued. However, conventional lithium-containing anode materials are unable to balance these two requirements, thereby necessitating the exploration of lithium-free anodes for SSBs. In the current study, a core–shell lithium-free α-Fe2O3@TiNb2O7 (TNO) nanofiber composite is synthesized and applied as an SSB anode. The confinement effect from the hollow TNO nanotubes on the encapsulated α-Fe2O3 nanoparticles can buffer the volume-change crushing during charging/discharging, leading to robust structural stability. Moreover, the high rate capability of TNO and high capacity of α-Fe2O3 work synergistically to provide superior electrochemical performances. The prepared α-Fe2O3@TNO composite delivers twice the reversible capacity (625 mA h g−1 at 0.1 A g−1) of pristine TNO as well as a remarkably prolonged cycle life (500 cycles with 79.2% capacity retention) and an improved rate performance (305 mA h g−1 at 3 A g−1) compared with those of α-Fe2O3, making this composite the most efficient TNO-based anode material ever reported. By pairing the composite with the high-energy Li[Ni0.8Co0.1Mn0.1]O2 (NCM811) cathode, the SSB full cell exhibits a high energy density of 400 W h kg−1. These results demonstrate the feasibility and great potential of the proposed lithium-free anode material in SSBs for practical applications.
研究领域:
材料科学
·
电化学
·
能源存储
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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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PubMed
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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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