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ADVANCED FUNCTIONAL MATERIALS · 2016 ·Vol. 27 ·期 4 ·1604258 · IF 11.382

MnO2 Gatekeeper: An Intelligent and O2-Evolving Shell for Preventing Premature Release of High Cargo Payload Core, Overcoming Tumor Hypoxia, and Acidic H2O2-Sensitive MRI

Zhifang Ma,Xiaodan Jia,Jing Bai,Yudi Ruan,Chao Wang,Jianming Li,Mengchao Zhang,Xiue Jiang

Premature leakage of photosensitizer (PS) from nanocarriers significantly reduces the accumulation of PS within a tumor, thereby enhancing nonspecific accumulation in normal tissues, which inevitably leads to a limited efficacy for photodynamic therapy (PDT) and the enhanced systematic phototoxicity. Moreover, local hypoxia of the tumor tissue also seriously hinders the PDT. To overcome these limitations, an acidic H 2 O 2 -responsive and O 2 -evolving core–shell PDT nanoplatform is developed by using MnO 2 shell as a switchable shield to prevent the premature release of loaded PS in core and elevate the O 2 concentration within tumor tissue. The inner core SiO 2 -methylene blue obtained by co-condensation has a high PS payload and the outer MnO 2 shell shields PS from leaking into blood after intravenous injection until reaching tumor tissue. Moreover, the shell MnO 2 simultaneously endows the theranostic nanocomposite with redox activity toward H 2 O 2 in the acidic microenvironment of tumor tissue to generate O 2 and thus overcomes the hypoxia of cancer cells. More importantly, the Mn(ΙΙ) ion reduced from Mn(ΙV) is capable of in vivo magnetic resonance imaging selectively in response to overexpressed acidic H 2 O 2 . The facile incorporation of the switchable MnO 2 shell into one multifunctional diagnostic and therapeutic nanoplatform has great potential for future clinical application.

研究领域: 生物医学工程 · 肿瘤治疗学 · 纳米医学
✓ 已验证 DOI 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Ni(OH)2 clusters decorated NiTiO3 Z-scheme heterojunctions with strong O2 activation and robust interfacial built-in electric field for efficient NO photo-oxidation

Guojun Li,Zheng Lian,Zhengwei Wan,Zhinian Liu,Jingwen Qian,Yue Deng,Shule Zhang,Qin Zhong

Photocatalytic oxidation offers a viable method for removing low-concentration NO from the atmosphere. However, poor oxygen adsorption-activation capacity and high re-combination rate of electrons and holes limit the photocatalytic NO oxidation activity. To over-come these problems, Ni(OH) 2 clusters decorated NiTiO 3 Z-scheme heterojunctions are constructed by a precipitation method. The tight interfacial contacts and built-in electric field between the (0   0   2) crystal facet of Ni(OH) 2 and (0   1   2) crystal facet of NiTiO 3 promote a Z-scheme charge transfer mechanism. This Z-scheme mechanism will enhance the charge-transfer driving force and result in high separation efficiency of the charges, thus leading to an enhanced photocatalytic performance. Importantly, introducing Ni(OH) 2 is considered a promising strategy to enhance the adsorption ability of the O 2 , NO and NO 2 . This might help to increase O 2 activation efficiency and speed up NO deep oxidation, leading to high NO removal efficiency and low NO 2 selectivity. Benefiting from the above excellent properties, the photocatalytic NO oxidation efficiency of Ni(OH) 2 /NiTiO 3 composites is enhanced and the formation of more toxic NO 2 is inhibited compared with that of NiTiO 3 . This work offers a promising and effective route to design efficient NiTiO 3 -based photocatalysts in the application of environmental remediation.

研究领域: 环境修复 · 光催化 · 材料科学 · 无机化学 · 空气污染控制
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JOURNAL OF HAZARDOUS MATERIALS · 2026 · IF 10.6

A Cr(VI)-free strategy through rapid-adsorption-and-strong-reduction in efficiently oxidative removal of Cr(III)-complexes by carbon-modified Al0/O2 system

Xinlei Zhang,Shiying Yang

The removal of hazardous Cr(III) complexes via advanced oxidation processes can generate highly toxic Cr(VI), posing significant environmental risks. Therefore, there is an urgent need to develop alternative methods that completely suppress the generation of Cr(VI). In this study, with no detectable Cr(VI) in the solution (below the detection limit of 0.004 mg/L), the carbon nanotubes-modified micron-sized zero-valent aluminum (CNTs@mAl 0 ) can effectively remove 99.50% of Cr(III)-EDTA and 83.34% of TOC under the typical acidic conditions of industrial chromium wastewater (pH = 3.00) by activating molecular oxygen. Then the following alkaline precipitation can easily remove the decomplexed free chromium, lowering total chromium concentration to 0.11 mg/L, which meets most national and regional standards, whereas direct alkali precipitation fails to meet them. Serving as a strong electron reservoir (E 0 = - 1.662 V), micron-sized zero-valent aluminum (mAl 0 ) synergizes with highly conductive carbon nanotubes (CNTs) to effectively activate O 2 , facilitating the production of reactive oxygen species (primarily 1 O 2 and •OH) that drive the oxidative decomplexation of Cr(III)-EDTA. Furthermore, the organic ligands are efficiently mineralized, thus preventing Cr(III)’s re-complexation. More interestingly, once the Cr(VI) is possibly generated, it would be rapidly absorbed by CNTs and be immediately reduced by mAl 0 with strong reducing power, thereby completely suppressing the generation of any Cr(VI) in bulk solution. In conclusion, this study presents an environmentally friendly and straightforward treatment system for Cr(III)-complexes, offering an effective solution to mitigate the environmental risks posed by chromium, particularly Cr(VI), in wastewater.

✓ 已验证 DOI PubMed 高影响因子
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ANALYTICAL CHEMISTRY · 2024 · IF 6.7

Silica Nanochannels as Nanoreactors for the Confined Synthesis of Ag NPs to Boost Electrochemical Stripping Chemiluminescence of the Luminol-O2 System for the Sensitive Aptasensor

Xiaoyu Zhou,Yanqi Zou,Hongjuan Ru,Fei Yan,Jiyang Liu

Herein, we, for the first time, synthesize silver nanoparticles (Ag NPs) within the nanochannels of amino group-functionalized vertically ordered mesoporous silica films (NH2–VMSF) and investigate their coreaction accelerator role in the luminol-dissolved oxygen (O2) electrochemical stripping chemiluminescence (ESCL) system. The synthesized Ag NPs are capable of electrocatalytic reduction of O2 to superoxide radicals, and meanwhile, sliver ions (Ag+) electrochemically stripped from Ag NPs can promote the amount of luminol anion radicals, generating the boosted ECL intensity of the luminol-dissolved O2 system. This proposed Ag NPs@NH2–VMSF on the indium tin oxide electrode was applied to construct the ESCL aptasensor for quantitative determination of prostate-specific antigen (PSA), yielding a low detection limit [0.19 pg/mL (S/N = 3)] and a broad linear dynamic range (1 pg/mL to 100 ng/mL). Furthermore, good analytical performance of PSA in serum with satisfactory recoveries and low relative standard deviation values is achieved by our developed ESCL aptasensor, rendering it a convenient and sensitive method for PSA determination in clinical applications and further broadening the strategy of ESCL techniques.

研究领域: 纳米技术 · 分析化学 · 生物传感器 · 电化学
✓ 已验证 产品关联 DOI PubMed 高影响因子
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Journal of Materials Chemistry A · 2018 ·Vol. 6 ·期 23 ·10856-10867 · IF 9.931

PdNi alloy decorated 3D hierarchically N, S co-doped macro–mesoporous carbon composites as efficient free-standing and binder-free catalysts for Li–O2 batteries

Xiangzhong Ren,Moujie Huang,Shan Luo,Yongliang Li,Libo Deng,Hongwei Mi,Lingna Sun,Peixin Zhang

A novel free-standing and binder-free air electrode with excellent electrochemical performance was designed for highly reversible Li–O2 batteries. The 3D hierarchically N, S co-doped macro–mesoporous carbon (NSMmC) was deposited on carbon paper (CP) via a template method, and then uniformly decorated with PdNi nanoparticles. The macropores of the porous carbon can provide enough space to accommodate discharge products, while the interconnected pores and channels efficiently facilitate oxygen and electrolyte diffusion. The introduction of PdNi nanoparticles greatly reduce the charge transfer resistance, resulting in the improvement of electron mobility of the whole cathode. Compared with Pd–NSMmC/CP and NSMmC/CP cathodes, the PdNi–NSMmC/CP cathode shows considerable enhancement of Li–O2 battery performance. The ultrafine and evenly distributed PdNi nanoparticles can not only provide enough catalytic sites, but can also tailor the discharge products into a cage-like morphology, which provides enough channels for electron and lithium ion transport. Moreover, the smaller size of the cage-like Li2O2 makes it decompose more easily, resulting in lower charge overpotential. This study provides a promising strategy to design 3D structured air cathodes for Li–O2 batteries with high electrocatalytic performance.

研究领域: 材料科学 · 电化学 · 能源存储 · 电池技术
✓ 已验证 产品关联 DOI 高影响因子
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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Promotion of O2 activation by ZIF-8 derived N-rich aluminum-graphite (Al-Gr-NPC) composite for non-radical degradation of antibiotic at neutral pH

Yufeng Da,Yong Liu,Yong Chen,Rui Han,Jianlong Wang

Recently, the activation of molecular oxygen (O 2 ) by graphite (Gr) supported aluminum (Al) composite for the in-situ generation of H 2 O 2 / OH gains increasing attention. However, the limited O 2 mass transfer and low catalytic activity of decomposition H 2 O 2 at neutral pH restrict its further application in the wastewater treatment. In this work, a novel N-rich graphite supported aluminum (Al-Gr-NPC) composite was fabricated by introducing the nitrogen-rich porous carbon (NPC) obtained from ZIF-8 derivative as precursor, and by a ball-milling and sintering process. The results showed that the NPC introduction not only improved the physiochemical property of Al-Gr, such as specific surface area, pore structure and hydrophobicity, facilitating the mass transfer of O 2 , but also made Al-Gr contain plentiful N species, serving as active sites for the two-electron ORR process and catalytic decomposition of H 2 O 2 . These excellent performances of Al-Gr-NPC favored the production and utilization of H 2 O 2 by the activation of O 2 at neutral pH and air aeration. The carbonization temperature of ZIF-8 determined the type of N species, surface area and the hydrophobicity of NPC. 1 O 2 was the main oxidant for tetracycline hydrochloride (TC) degradation. 100 % TC degradation and 60.57 % of TOC removal were achieved within 60 min at neutral pH, Al-Gr-NPC dosage of 0.5 g/L and initial TC concentration of 20 mg/L. The toxicity of the final products of TC degradation were much lower than TC by ECOSAR software analysis. Al-Gr-NPC could be used for the removal of antibiotic contaminants from wastewater.

✓ 已验证 产品关联 DOI 高影响因子
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JOURNAL OF HAZARDOUS MATERIALS · 2022 · IF 14.224

New insight of zero-valent iron activation S(IV) in absence of external hydrogenation ions for decomposing micropollutants: Two radical generation pathways depending on O2

Tong Liu,Yang Liu,Peng Zhou,Zhaokun Xiong,Heng Zhang,Chuanshu He,Ye Du,Gang Yao,Bo Lai

As one of the most promising advanced oxidation processes , the activation of S(IV) by iron-based materials to produce SO 4 •− has become a hot technology for the degradation of organic pollutants . However, the mechanism of radical chain reactions has not been clearly explored. Herein, we established a novel AOP system based on the combination of zero-valent iron (ZVI) and potassium pyrosulfite (PPS). Combined with the degradation trends of CBZ and the change of DO concentration, the system was proposed to be divided into a slow initiation stage in 5 min and a rapid degradation stage in 5 − 10 min. Through a series of quenching experiments, electron paramagnetic resonance tests and several probe experiments, the mechanisms of two radical chain reactions were proposed between ZVI and PPS: the first one produced O 2 •− and HO • , and the other produced SO 3 •− , SO 5 •− , SO 4 •− and HO • . The two-stage reaction and two radical production paths of the ZVI/PPS system were proposed for the first time, which provided theoretical guidance for the practical application of the ZVI/PPS system. The ZVI/PPS system has been found to have excellent environmental adaptability in the treatment of industrial wastewater .

✓ 已验证 产品关联 DOI 高影响因子
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VACUUM · 2023 · IF 4

Enhanced photocatalytic degradation of EMPs by hydrogenation modified different morphologies α-Fe2O3-x

Chaoqun Yan,Zhiliang Cheng,Xuan Zhang,Juan Wei,Qian Xu

The photocatalytic efficiency of hematite (α-Fe 2 O 3 ) is limited by its photoexcited state lifetime and diffusion length. By adjusting the surface structure, the photogenerated electron pairs can migrate to the surface and the charge recombination can be suppressed, which can effectively solve these problems and improve the photo-Fenton performance. In this study, four kinds different morphologies of α-Fe 2 O 3 - x (truncated hexagonal bipyramidal, cubic, hexagonal shape, and spherical) were synthesized by hydrothermal method , and a photocatalyst (H-α-Fe 2 O 3 - x ) with higher catalytic activity was prepared by hydrogenation. The results of UV–Vis DRS , PL , Raman, and XPS analysis , the oxygen vacancies and Fe (II) species were introduced into the α-Fe 2 O 3 catalyst after the hydrogenation reaction. The H-α-Fe 2 O 3 - x showed good degradation performance for TC and DX as EMPs model pollutants. The results show that the formation of oxygen vacancy and Fe 2+ is the main factor to improve the photocatalytic activity of the reaction system. Furthermore, the reaction mechanism revealed that reactive radicals involved in the H-α-Fe 2 O 3 - x photocatalytic system were •OH, •O 2 − , and h   +  responsible. This study provides an alternative technology for an easy and effective means for bandgap engineering to improve the photocatalytic performance of photocatalysts and facilitate widening environmental application.

研究领域: 环境科学 · 材料科学 · 化学 · 光催化
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ACS Applied Materials & Interfaces · 2021 · IF 9.229

Revealing the Local Cathodic Interfacial Chemism Inconsistency in a Practical Large-Sized Li–O2 Model Battery with High Energy Density to Underpin Its Key Cyclic Constraints

Gangning Zhang,Shigang Lu,Shangqian Zhao,Li Zhang,Haobo Sun

Due to the theoretical ultrahigh energy density of the Li–O2 battery chemistry, it has been hailed as the ultimate battery technology. Yet, practical Li–O2 batteries usually need to be designed in a large-sized pattern to actualize a high specific energy density, and such batteries often cannot be cycled effectively. To understand the inherent reasons, we specially prepared large-sized (13 cm × 13 cm) Li–O2 model batteries with practical energy output (6.9 Ah and 667.4 Wh/kgcell) for investigations. By subregional and postmortem analysis, the cathode interface was found to have severe local inhomogeneity after discharge, which was highly associated with the electrolyte and O2 maldistribution. The quantitative results by X-ray photoelectron spectroscopy (XPS) evidenced that this local inhomogeneity can exacerbate the generation of lithium acetate during charge, where the locally higher ratio of unutilized carbon surface and less Li2O2 after discharge would result in increased lithium acetate formation for a subsequent local overcharge. Moreover, verification experiments proved that the byproduct lithium acetate, which had been of less concern, was recalcitrant and triggered much larger polarization compared with the commonly reported byproduct Li2CO3 during battery operations, further revealing the key limiting factors leading to the poor rechargeability of batteries by its accumulation at a pouch-type cell level.

研究领域: 材料科学 · 电化学
✓ 已验证 DOI PubMed 高影响因子
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JOURNAL OF POWER SOURCES · 2019 · IF 7.467

InBr3 as a self-defensed redox mediator for Li–O2 batteries: In situ construction of a stable indium-rich composite protective layer on the Li anode

Jia Liu,Tong Wu,Siqi Zhang,Dan Li,Ying Wang,Haiming Xie,Jinghai Yang,Guiru Sun

One big obstacle for a redox mediator (RM)-based Li–O 2 system is the redox shuttling between the diffusible RM + and Li anode, leading to the unexpected RM degradation and continuous deterioration of Li anode, which inevitably results in a low energy efficiency and a poor cycling stability for the Li–O 2 battery. Here, InBr 3 as a self-defensed RM is firstly introduced into Li–O 2 batteries, which can lower the cell overpotential and thus improve the cycling performance. Moreover, due to the In 3+ existence, an In-rich composite protective layer can be in situ generated on the Li anode, which contributes to suppressing the redox shuttling, improving the interface stability of Li and electrolyte, and inhibiting the dendrite formation. This work gives an insight into the development of self-defensed RM and the protection of the Li anode for Li–O 2 batteries.

研究领域: 储能 · 电化学 · 材料科学 · 电池技术
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Catalysts · 2026 ·Vol. 16 ·期 5 ·417 · IF 4.5

Alkali Metal-Promoted Au/TS-1 Bifunctional Catalyst for Highly Efficient and Stable Gas-Phase Propylene Epoxidation with H2 and O2 via In Situ-Generated H2O2

Ziyan Mi,Huayun Long,Yuhua Jia,Yue Ma,Cuilan Miao,Yan Xie,Xiaomei Zhu,Jiahui Huang

Developing effective catalysts for the epoxidation of propylene with H2and O2holds significant scientific and industrial significance. This study synthesized a series of Au/TS-1 catalysts modified with alkali metals (Na+, Cs+) and carefully examined their impact on gas-phase propylene epoxidation, with particular attention to the role of anions. The optimal Au–CsC(1:10)/TS-1 catalyst (Cs2CO3modified, Au/Cs molar ratio = 1:10) achieves a propylene conversion of 16.8%, a PO selectivity of 88.5%, an H2efficiency of 40.8%, a record PO formation rate of 383.9 gpo·kgcat−1·h−1, and unprecedented long term stability (>380 h without deactivation). To the best of our knowledge, no previous study has simultaneously achieved such balanced and outstanding performance across all these key indicators. Comprehensive characterization reveals that Cs+modification suppresses side reactions and coke formation, increases microporosity, tunes surface acid–base properties and hydrophobicity, restricts Au particle size, and stabilizes both Au0and tetra coordinated Ti sites, thereby inhibiting H2O2decomposition and PO isomerization while greatly enhancing reaction efficiency. This holistic advancement represents a significant leap forward for Au based catalysts in gas phase propylene epoxidation, offering both a theoretical foundation and practical guidance for the development of high performance epoxidation catalysts.

✓ 已验证 DOI 高影响因子
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ANALYTICAL CHEMISTRY · 2026 · IF 7.3

Glucose/O2 Enzymatic Biofuel Cell Constructed with a Laccase-Mimicking Nanozyme for Efficient Cathode Oxygen Reduction and Bacterial Surface-Displayed Cascade Enzymes for an Anode Biocatalyst

Yuhan Chen,Boyan Wang,Yafei Du,Yaru Zhang,Ying Zhang,Lu Bai,Serge Cosnier,Bo Liang,Aihua Liu

Enzymatic biofuel cell (EBFC) is an electrochemical device that uses enzymes to convert the chemical energy of renewable biomass into electrical energy. However, improving the EBFC performance, such as the cost-effectiveness, operational stability, output power density (Pmax), and open circuit voltage (OCV), remains challenging. Especially, the activity and stability of enzymes, substrate tolerance, cost, and immobilization strategy are crucial in developing EBFCs. Herein, we report on MnO2 nanosheets (MnO2 NSs) prepared via facile chemical precipitation, exhibiting outstanding laccase-mimicking activity with good stability and excellent resistance to halide ions. Then, for the first time, the laccase-like nanozyme could replace natural laccase as a cathode catalyst for efficient oxygen reduction reaction under nearly neutral pH condition, which exhibits an onset potential of 841 mV vs NHE in O2 reduction mediated by 2,2-bisazo-bis(3-ethyl-benzothiazole-6-sulfonic acid) diammonium salt. In addition, cascade enzymes of polyphosphate glucokinase (PPGK) and glucose 6-phosphate dehydrogenase (G6PDH) were successfully displayed on the Escherichia coli (E. coli) surface. The resultant PPGK-E. coli can catalyze the oxidation of glucose to glucose-6-phosphate (G6P), which can be subsequently oxidized by G6PDH-E. coli in the presence of the coenzyme NAD+ efficiently and converted to NADH. Finally, a dual-chamber glucose/O2 EBFC was constructed with PPGK-E. coli/G6PDH-E. coli (2:1) as the anodic catalyst and an MnO2 NS-based cathodic catalyst. The bacterial surface-displayed enzymes were kept in an anodic solution, which could not only retain the enzyme activity but also ensure mass transfer efficiency, thereby greatly enhancing the enzyme's inherent catalytic potential. The as-developed EBFC achieved an OCV of 0.68 V and a Pmax of 32.2 μW/cm2 as well as good operational stability. The strategies proposed provide new ideas for constructing high-performance EBFCs using other nanozymes and biocatalysts, which may provide new avenues for the development and utilization of sustainable energy for promising applications in wearable devices or in self-powered sensors.

✓ 已验证 DOI PubMed 高影响因子
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