CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Jialong Yin,Heng Zhang,Mengfan Luo,Jia Zhao,Bingkun Huang,Pinji Chen,Zhenpeng Cai,Yue Yuan,Yang Liu,Chuanshu He,Bo Lai
The ferrous species (Fe(II))-periodate (PI) system employs efficient decontamination by generating ferryl species (Fe(IV)-oxo) under acidic pH conditions. However, the mechanisms by which the Fe(II)/PI system operates across a broad pH range remain elusive. In light of the rapid oxidation and consumption of Fe(II) at neutral pH, we developed an electro-Fe(II) system utilizing an iron plate anode to activate PI (E(Fe/C)/PI). Efficient sulfamethoxazole (SMX) degradation was achieved under the E(Fe/C)/PI system across a range of pH values. Quenching and chemical probe experiments revealed a transition from Fe(IV)-oxo to singlet oxygen ( 1 O 2 ) as the predominant reactive species from acidic to near-neutral pH, respectively. Density functional theory (DFT) calculations indicated that the differences in one-electron transfer capacity and hydrolysis pathways for various protonated Fe(IV)-oxo species underlie the variations in catalytic mechanisms. This study not only enhances the efficiency of the Fe(II)/PI system but also provides a comprehensive understanding of the activation mechanisms at different pH levels.
研究领域:
环境化学
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电化学
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催化
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水处理
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产品关联
DOI
高影响因子
ACS Catalysis
·
2021
·
IF 13.084
Lipeng Wu,Bin Li,Yang Li,Xiaobin Fan,Fengbao Zhang,Guoliang Zhang,Qing Xia,Wenchao Peng
Herein, a series of Co@N–C materials are synthesized using nitrates (LiNO3, NaNO3, and KNO3) as templates to control the preferential growth of the cobalt (200) facet. Co@N–C–X (X = LiNO3, NaNO3, and KNO3) exhibit excellent activities and long-term stabilities for Fenton-like degradation of bisphenol A (BPA) with peroxymonosulfate (PMS) as an oxidant. The texture coefficient (TC) is used to investigate the relationship between the Co facets and their catalytic activities, and a linear relation is built between the TC of Co(200) and the reaction rate constant (k). Co(200) is therefore the most active facet for PMS activation, while nitrates can promote the preferential growth of the Co(200) facet. Moreover, the Co(200) facet is more stable against leaching and can achieve more quick transformation between Co2+/Co3+. Quenching tests, electron paramagnetic resonance spectra, and electrochemical tests show that singlet oxygen (1O2) plays the dominant role for BPA degradation. Density functional theory verifies that Co nanoparticles coated with a graphitic nitrogen-doped carbon layer have the best activity for PMS activation. This work first proposes the strategy of using nitrates to control the preferential growth of Co facets and reveals the relationship between the TC value and k, thus attracting great interest in the environmental field.
研究领域:
环境科学
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催化
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材料科学
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产品关联
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2025
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IF 7.7
Yuantian Zhao,Zhiwei Zhou,Haikuan Yu,Xing Li,Jiawei Ren,Junyan Chen,Fei Qi
Developing carbonaceous composites with strong non-radical activity and recyclability is key for sustainable wastewater purification. Herein, a novel photocatalytic process was designed using zinc ferrite loaded on oxalic acid-modified powdered activated carbon (ZFO/OA/PAC) to activate persulfate (PDS) under visible light (VL) irradiation. ZFO was in-situ grown onto OA/PAC via C=O bridging, forming stable Zn/Fe–O–C bonds that suppressed magnetic agglomeration and enabled directional electron transfer. The optimized interfacial binding energy of 22.45 kcal/mol reduced the activation energy barrier, enhancing active site utilization and reaction kinetics through efficient electron cycling. With a narrow bandgap of 1.54 eV, 0.1 g/L ZFO/OA/PAC and 0.1 g/L PDS achieved 94.3% tetracycline (TC) removal under VL, with a kinetic constant 23.75 times higher than pristine ZFO. The process predominantly generated h + and 1 O 2 , the latter arising from superoxide conversion, PDS-induced functional group transformation, and oxygen-vacancy-mediated electron transfer. Photocatalysis also promoted Fe(III)/Fe(II) cycling, further aiding reactive oxygen species (ROS) formation. Seventeen intermediates were identified, with degradation and detoxification proceeding mainly through ring-opening, substitution, and ROS-driven molecular reconstruction. The magnetic ZFO/OA/PAC exhibits broad organic pollutants’ removal capability and effective adaptability to real water matrices. This work provides a paradigm for designing magnetic carbonaceous photocatalysts to leverage non-radical pathways, advancing scalable wastewater purification technologies.
研究领域:
环境科学
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材料科学
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化学工程
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光催化
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水处理技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry B
·
2021
·Vol. 9
·期 26
·5255-5263
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IF 6.331
Jiansheng Liu,Xueqin Qing,Qin Zhang,Ningyue Yu,Mengbin Ding,Zhaohui Li,Zhen Zhao,Zhiling Zhou,Jingchao Li
Photodynamic therapy (PDT) has provided a promising approach for the treatment of solid tumors, while the therapeutic efficacy is often limited due to the hypoxic tumor microenvironment, resulting in tumor metastasis. Herein, we report an oxygen-producing proenzyme hydrogel (OPeH) with photoactivatable enzymatic activity for PDT enabled metastasis-inhibiting combinational therapy of breast cancer. This OPeH based on alginate is composed of protoporphyrin IX (PpIX) conjugated manganese oxide (MnO2) nanoparticles, which act as both the photosensitizer and oxygen-producing agent, and singlet oxygen (1O2)-responsive proenzyme nanoparticles. In the hypoxic and acidic tumor microenvironment, MnO2 can generate 1O2 to promote PpIX-mediated PDT with an amplified 1O2 generation efficiency, which also triggers the cleavage of 1O2-responsive linkers and cascade activation of proenzymes for cancer cell death. This combinational therapy upon photoactivation not only greatly inhibited the tumor growth, but also suppressed lung metastasis in a mouse xenograft breast tumor model, which is impossible in the case of PDT alone. This study thus provides a proenzyme hydrogel platform with photoactivatable activity for metastasis-inhibiting cancer therapy with high efficacy and safety.
研究领域:
癌症治疗
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纳米医学
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生物医学工程
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肿瘤微环境研究
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产品关联
DOI
PubMed
高影响因子
ChemistrySelect
·
2024
·Vol. 9
·期 8
·e202303088
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IF 1.9
Xiayan Zhang,Zhi Song,Boxia Liu,Jialu Liu,Yeqiong Huang,Dongxu Han
Graphical Ni/Fe bimetallic atom cluster catalyst is prepared by a hydrothermal to stimulate PMS to produce high concentration 1 O 2 and efficiently remove BPA from aqueous solution. It is found that 1 O 2 in the system is the most important active component in the degradation process of BPA, and a high concentration of 1 O 2 could promote the rapid degradation of BPA in solution. The advanced oxidation process based on peroxymonosulfate (PMS) is a new water purification strategy. In this work, Ni/Fe bimetallic atom cluster composite catalyst is prepared by a hydrothermal synthesis to stimulate PMS to produce high concentration singlet oxygen ( 1 O 2 ) and efficiently remove bisphenol A (BPA) from aqueous solution. The experimental data show that in a broad pH range (pH=3–11), the removal rate of BPA by the non-free radical pathway induced by 1 O 2 is close to 100 %, and the catalyst still has high stability after 5 cycles. The mechanism of BPA removal in NiFe−BC/PMS/BPA catalytic degradation system is investigated by quenching experiment. It is found that 1 O 2 in the system is the most important active component in the degradation process of BPA, and a high concentration of 1 O 2 could promote the rapid degradation of BPA in solution. In this paper, the high catalytic activity and selectivity of bimetallic atomic cluster catalysts can provide new insights for the treatment of phenolic wastewater.
研究领域:
环境科学
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催化
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水处理
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Shihua Zhang,Shuang Dai,Qiao Huang,Jincan Huang,Shengqiang Hei,Peng Wang,Biming Liu
The confinement effect triggered by nano-confinement systems in the advanced oxidation processes has received extensive attention. In this study, the strategy of constructing stable confined Co 3 O 4 @SiO 2 materials and activating peroxymonosulfate (PMS) was adopted to successfully achieve the efficient removal of enrofloxacin (EON). The removal efficiency of EON by Co 3 O 4 @SiO 2 (0.08 g/L) could reach 99 % at pH 0 of 7 and PMS of 0.2 g/L, and the optimal degradation rate could reach 0.147 min −1 , which was 9.6 times higher than that of the unconfined system. The reaction process was mainly driven by the synergistic interaction between the non-radical 1 O 2 and the interfacial electron transfer network, and the formation of oxygen vacancies within the reaction system accelerated the degradation process. Density functional theory calculations further showed that the confinement effect of SiO 2 aerogel stabilized the Co 3 O 4 nanoparticles, the charge transfer efficiency between Co 3 O 4 @SiO 2 and PMS was optimized, and at the same time, Co 3 O 4 was the key active site for EON degradation. This research can provide an effective strategy for the activation of PMS by SiO 2 aerogel confined structure to remove antibiotic pollutants.
研究领域:
环境科学
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材料化学
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高级氧化过程
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纳米材料
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污染物降解
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产品关联
DOI
高影响因子
JOURNAL OF NANOBIOTECHNOLOGY
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2025
·Vol. 23
·期 1
·1-23
·
IF 12.6
Zou Lan,Wang Rujing,Zhao Mengnan,Li Yuke,Sun Chen,Xie Jinjin,Chen Yan,Jing Qian,Mi Dandan,Shi Sanjun
Pyroptosis, a recently identified cellular demise regulated by gasdermin family proteins, is emerging as a promising avenue in cancer immunotherapy. However, the realm of light-controlled pyroptosis in cancer cells remains largely unexplored. In this study, we took a deliberate approach devoid of any chemical alterations to develop a novel photosensitizer called “pharmaceutical-dots (pharm-dots)” by combining nonemissive polymers (Poly (lactic-co-glycolic acid), PLGA) with nonfluorescent invisible molecules like curcumin, berberine, oridonin into PLGA nanoparticles (PLGA-NPs). Initially, our research commenced with a comprehensive mechanistic comparison study, consolidating fragmented information on optical mechanisms. This exploration revealed that surface passivation atoms play a dominant role in governing the fluorescence emission of PLGA-NPs. Remarkably, these new luminophores, composed of two non-inherently luminous components, exhibit a remarkable synergistic boost in photoluminescence through a “0 + 0 > 2” phenomenon. In-depth investigations uncovered that these luminous PLGA-NPs, capable of generating 1 O 2 , induce pyroptosis under photoexcitation conditions through the caspase-3/gasdermin E (GSDME) pathway. Simultaneously, our findings highlight PLGA-NPs as a novel optical formulation suitable for imaging, displaying substantial biological activity when paired with photoirradiation. This discovery holds the potential to facilitate the application of light-controlled pyroptosis in antitumor therapy, marking a promising stride toward innovative approaches in cancer treatment. Graphical abstract
研究领域:
癌症研究
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生物光子学
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纳米技术
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免疫疗法
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分子生物学
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产品关联
DOI
PubMed
高影响因子
Environmental Science-Nano
·
2020
·Vol. 7
·期 10
·2982-2994
·
IF 7.683
Weijian Duan,Jinglei He,Ziliang Wei,Zongren Dai,Chunhua Feng
The heteroatom-doped, carbon-activated peroxymonosulfate (PMS) system proceeding via the non-radical oxidation pathway involving singlet oxygen (1O2) represents a promising advanced oxidation process (AOP) due to the resistance of 1O2 to background anions in solution. However, the performance level of pollutant removal is not yet satisfied, and the mechanism of 1O2 generation remains elusive. Herein, we report the development for the first time of a unique Si-engaged heteroatom (i.e., N)-doped carbon (Si/N–C) nanomaterial for PMS activation, which exhibits outstanding performance in the removal of various kinds of pollutants and an appreciably wide working pH range of 2.5 to 11. Taking rhodamine B (RhB) as an example, the Si/N–C@PMS system achieved a much higher reaction rate (0.64 min−1) than the Si–C (0.047 min−1), N–C (0.017 min−1), SiO2 (0.021 min−1), and Co3O4 (0.026 min−1; a standard catalyst) systems. In addition, the results of electron spin resonance (ESR) and scavenging experiments solidly support the conclusion that the mechanism of 1O2 generation in this system is via the recombination of superoxide radicals O2˙−, a pathway seldom reported for metal-free, catalyst-activated PMS systems. More importantly, we observed apparent inhibition effects of the anions (e.g., HCO3−, HPO42−, and PO43−) on the degradation performance, inconsistent with many previous reports suggesting that the 1O2-mediated oxidative system possesses a high selectivity toward pollutant degradation in the presence of these anions. Further studies with the anions, including Cl−, HCO3−, and HxPO4(3−x) (x = 0, 1, 2), suggest that the reaction between O2˙− and these anions is the main reason for the abnormal salt effect. This work will deepen the understanding of 1O2 formation via the intermediate of O2˙− and provide a new insight into its salt resistance capacity.
研究领域:
环境化学
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材料科学
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催化
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水处理
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DOI
高影响因子
BIOMATERIALS
·
2020
·
IF 10.317
Jing Yan,Qinghua Wu,Ziyin Zhao,Jianhua Wu,Huan Ye,Qiujun Liang,Zhuchao Zhou,Mengying Hou,Xudong Li,Yong Liu,Lichen Yin
The anticancer performance of nanomedicine is largely impeded by insufficient intratumoral penetration. Herein, tumor microenvironment (TME)-amendatory and self-adaptive nanoclusters (NCs) capable of cancer-associated fibroblasts (CAFs) depletion and size/charge conversion were engineered to mediate light-assisted, hierarchical intratumoral penetration. Particularly, large-sized NCs (~50 nm) were prepared via self-assembly of FAP-α-targeting peptide-modified, 1 O 2 -sensitive polymers, which were further used to envelope small-sized dendrimer (~5 nm) conjugated with Ce6 and loaded with DOX (DC/D). After systemic administration, the NCs efficiently targeted CAFs and generated lethal levels of 1 O 2 upon light irradiation, which depleted CAFs and concomitantly dissociated the NCs to liberate small-sized, positively charged DC/D. Such stroma attenuation and NCs transformation collectively facilitated the delivery of DC/D into deeper regions of CAF-rich tumors, where DOX and 1 O 2 provoked synergistic anti-cancer efficacies. This study provides an effective approach to facilitate the tumor penetration of nanomedicine by concurrently and spatiotemporally reconfiguring the nano-properties and remodeling the TME.
研究领域:
纳米技术
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癌症治疗
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药学
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生物医学工程
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Caiyun Xu,Junqin Li,Chunlei Ou,Jing Yang,Shuting Fu,Weiqing Hu,Li Wang,Zefeng Wang,Luo Hai,Le Deng,Dinggeng He
Chemodynamic therapy (CDT) involving highly toxic hydroxyl radical (•OH) with no drug resistance has gained widespread attention for antibacterial applications. However, the CDT effect is seriously confined by overexpressed glutathione (GSH) and limited hydrogen peroxide (H 2 O 2 ) in the infection sites. Here, we have constructed a cascade enzyme/nanozyme assembly (MCS/GOx) composing of a bimetallic sulfide MoCuS x (MCS) nanozyme loaded with natural glucose oxidase (GOx) for synergistic photothermal/photodynamic enhanced chemodynamic antimicrobial therapy with high performance. The loaded GOx can promote the peroxidase (POD)-like activity of MCS by providing an acidic microenvironment and self-supplying H 2 O 2 , achieving cascade generation of •OH for efficient CDT. The CDT effect can be further promoted by a co-catalysis mediated by the Mo 4+ /Mo 6+ redox couple. Upon exposure to an 808 nm near-infrared laser, MCS/GOx provides hyperpyrexia for photothermal antibacterial therapy (PTT), and produce singlet oxygen ( 1 O 2 ) for photodynamic therapy (PDT). Moreover, MCS/GOx can significantly consume antioxidant glutathione via the Cu + /Cu 2+ redox couple and PDT-mediated 1 O 2 production, thereby enhancing CDT antibacterial effect. In vitro experiments exhibit that MCS/GOx has combined antimicrobial effect against Staphylococcus aureus and Escherichia coli . Further in vivo studies demonstrate that MCS/GOx can efficiently eliminate bacterial cells in wound tissues and accelerate wound healing with low inflammatory response and good biosafety. Consequently, the proposed MCS/GOx with multiple bactericidal modalities shows a great potential in fighting wound infections.
研究领域:
纳米技术
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生物医学工程
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材料科学
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药学
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细菌学
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产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 42
·16119-16125
·
IF 4.569
Shengnan Liu,Jiahong Han,Weijin Wang,Yulei Chang,Runlin Wang,Ziwei Wang,Guangzhe Li,Dongxia Zhu,Martin R. Bryce
Photodynamic therapy (PDT) is a promising cancer treatment method. Traditional small-molecule photosensitizers (PSs) suffer from low intersystem crossing (ISC) ability and aggregation-caused quenching (ACQ), which adversely affects the luminous efficiency and singlet oxygen (1O2) yield of PSs in the aggregated state. Ir(III) complexes are promising PSs with long excited-state lifetime, good photophysical and photochemical properties and large Stokes shifts. Aggregation-induced emission (AIE) characteristics could reduce the nonradiative recombination and improve the ISC ability of excited states through the restriction of the intramolecular motions in aggregated states. Accordingly, two AIE-active Ir(III) complexes Ir-1-N+ and Ir-2-N+ were successfully designed and obtained based on Schiff base ligands. Experimental results showed that Ir-1-N+ and Ir-2-N+ have good photophysical properties and the corresponding nanoparticles (NPs) have good water solubility and 1O2 generation ability. Notably, Ir-2-N+ NPs can be efficiently taken up by mouse breast cancer cells (4T1 cells) with good biocompatibility, low dark toxicity and excellent phototoxicity. This work demonstrates a versatile strategy for exploiting efficient transition metal PSs with a cationic ligand in PDT.
研究领域:
化学
·
材料科学
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生物医学工程
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癌症研究
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Wensong Zou,Jing Li,Ranhao Wang,Jingyi Ma,Zhijie Chen,Lele Duan,Hongwei Mi,Hong Chen
Herein, we converted spent LiFePO 4 battery to the sea urchin-like material (SULM) with a highly efficient and environment-friendly method, which can contribute to building a zero-waste city. With SULM as a Fenton-like catalyst, a highly-efficient degradation process was realized for organic pollutants with interface and solution synergistic effect. In our SULM+NH 2 OH+H 2 O 2 Fenton-like system, NH 2 OH can effectively promote the interface iron ( Fe(Ⅲ)/ Fe(Ⅱ)) and solution iron (Fe(Ⅲ)/Fe(Ⅱ)) redox cycle, thus promoting the generation of reactive oxygen species (ROS). However, the ROS generation process and organic pollutants degradation pathway with the presence of NH 2 OH remains a puzzle. Here the detailed ROS generation mechanism and pollutants degradation pathway have been illustrated carefully based on experimental exploration and characterization. Therein, hydroxyl radicals (·OH) and singlet oxygen ( 1 O 2 ) are the main ROS for oxidizing and degrading organic pollutants. Notably, 1 O 2 can be converted from superoxide radicals (·O 2 ) in SULM+NH 2 OH+H 2 O 2 system. This study not only demonstrates the strategy of "trash-to-treasure" and "waste-to-control-waste" to simultaneously reduce the hazardous release from industrial solid waste and organic wastewater, it also provides new mechanistic insights for NH 2 OH mediated Fenton-like redox system.
研究领域:
环境科学
·
材料科学
·
化学工程
·
废物管理
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）