Nanoscale
·
2024
·Vol. 16
·期 22
·10727-10736
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IF 5.8
Peijiao Chen,Zhijun Li,Pengze Wang,Yuxin Yao,Tianwei Dou,Yang Qu,Liqiang Jing
The photocatalytic water-mediated CO2 reduction reaction, which holds great promise for the conversion of CO2 into valuable chemicals, is often hindered by inefficient separation of photogenerated charges and a lack of suitable catalytic sites. Herein, we have developed a glycerol coordination assembly approach to precisely control the distribution of atomically dispersed Cu species by occupying Ti-defects and adjusting the ratio between Cu species and Ti-defects in a hierarchical TiO2. The optimal sample demonstrates a ∼4-fold improvement in CO2-to-CO conversion compared to normal TiO2 nanoparticles. The high activity could be attributed to the Ti defects, which enhance the photogenerated charge separation and simultaneously facilitate the adsorption of water molecules, thereby promoting the water oxidation reaction. Moreover, by means of in situ EPR and FTIR spectra, we have demonstrated that Cu species can effectively capture photogenerated electrons and facilitate the adsorption of CO2, so as to catalyze the reduction of CO2. This work provides a strategy for the construction of atomic-level synergistic catalytic sites and the utilization of in situ techniques to reveal the underlying mechanism.
研究领域:
材料科学
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环境科学
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化学
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DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
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2024
·
IF 7.4
Jieli Ou,Yiqing Liu,Linyue Zhang,Zhenran Wang,Yuqi Tang,Yongsheng Fu,Dandan Zhao
Although Cu(II)/peroxymonosulfate (PMS) process has been successfully applied to degrade varied organic contaminants in water, the slow transformation of Cu(II) to Cu(I) that works only in alkaline conditions retards the treatment efficiency of this process. In this study, a new finding was observed, that is, oxytetraczdycline (OTC) could effectively enhance the degradation of organic pollutants in Cu(II)/PMS process where it was also removed in acidic conditions. With the addition of OTC in Cu(II)/PMS system, 85.5% of rhodamine B (RhB) was degraded in 90 min at pH 4.0, which was far more than that without OTC (36.1%), and simultaneously 98.1% of OTC was eliminated. The added OTC could form OTC-Cu(II) complexes which might powerfully improve the reduction of Cu(II) to Cu(I), exerting a positive effect on the PMS activation and subsequent degradation of RhB. Electron paramagnetic resonance (EPR) experiments assisted with radical scavenging experiments and Raman spectrum detection results suggested that Cu(III) and hydroxyl radical (HO • ) were the predominant reactive species for RhB degradation, while OTC removal in this system was mainly ascribed to direct PMS oxidation. The Cu(II)/PMS process also showed a promising success on the synergistic degradation of OTC with the other four refractory organic pollutants , indicating the potential application of PMS oxidation in water treatment .
研究领域:
环境科学
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水处理工程
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DOI
高影响因子
Journal of Cleaner Production
·
2024
·
IF 9.7
Jinling He,Shuman Huang,Nan Jiang,Ai Zhang,Andere Clement Miruka,Yanan Liu,Xiang Li,Pin Gao,Gang Xue
The use of waste activated sludge (WAS) fermentative short-chain fatty acids (SCFAs) as the excellent carbon source of wastewater biological nutrient removal has drawn much attention recently as it can reuse WAS organics and reduce WAS production. This study developed a novel, efficient, and environmentally friendly approach combining atmospheric pressure plasma jet with microbubbles (plasma/MBs) for WAS pretreatment. Compared with the control, plasma/MBs pretreatment enhanced SCFA generation by 92% and acetic acid proportion by 21% with plasma discharge power at 500 W and MBs dosage at 7.9 mg/L dissolved oxygen. The plasma/MBs combination motivated the reaction of various reactive species (such as O 3 , NO x , ONOO − , •OH, e − , 1 O 2 , and •O 2 − ) and enhanced the activity of physical energies (such as light and heat). This synergy promoted sludge cell lysis and biodegradable substance release, significantly boosting acetic acid-enriched SCFA generation from fermentation. Moreover, plasma/MBs pretreatment increased the expression of key genes for SCFA production during fermentation, which also contributed to the production of SCFAs. Besides, plasma/MBs pretreatment favored WAS dewatering, heavy metal removal, and organic pollutant degradation, providing a new approach to advancing WAS resource recovery through innocuous management.
研究领域:
环境工程
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生物技术
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微生物学
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污水处理
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DOI
高影响因子
Small
·
2024
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IF 13
Yi Shen,Yongliang Pan,Chao Zhu,Haizhong Zhang,Jun Wang,Renlan Liu,Qile Fang,Shuang Song,Baoliang Chen
In the domain of heterogeneous catalytic activation of peroxymonosulfate (PMS), high-valent metal-oxo (HVMO) species are widely recognized as potent oxidants for the abatement of organic pollutants. However, the generation selectivity and efficiency of HVMO are often constrained by stringent requirements for catalyst adsorption sites and electron transfer efficiency. In this study, a single-atom catalyst, Cu SA /CN P&S, is synthesized featuring multiple types (planar/axial) of heteroatom coordination via an H-bond-assisted self-assembly strategy. It is confirmed that CuN 3 active centers with axial S coordination are uniformly distributed in a carbon matrix modified by planar P atoms. Cu SA /CN P&S activated PMS to selectively generate Cu (III) ═OH species as the primary reactive oxygen species (ROS). The pseudo-first-order kinetic rate for bisphenol A degradation reached 1.51 min −1 , a 17.57-fold increase compared to the unmodified Cu SA /CN catalyst. Additionally, the Cu SA /CN P&S catalyst demonstrates high efficiency and durability in removing contaminants from various aqueous matrices. Theoretical calculations and experimental results indicate that the intrinsic electric field generated by distal planar P atoms enhances electron transfer efficiency within the carbon matrix. Meanwhile, axial S coordination elevates the d-band center and tunes the e g * band broadening of Cu, thereby enhancing the adsorption selectivity for the terminal oxygen of PMS. This multitype coordination synergistically mitigates the issues of low selectivity and yield of HVMO species.
研究领域:
环境科学
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催化化学
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材料科学
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DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2025
·
IF 8.5
Chaofan Yao,Qian Wu,Yu Zhao,Hongbin Li,Jinmei He,Li Liu,Yudong Huang,Feng Cheng
Wound bacterial infections not only impede the healing process but can also give rise to a range of serious complications, thereby posing a substantial risk to human health. Developing effective wound dressings incorporating phototherapy functionalities, specifically photothermal therapy (PTT) and photodynamic therapy (PDT), remains a critical area of research in modern wound care. Existing PTT-PDT systems often suffer from challenges such as nanoparticle aggregation and inefficient reactive oxygen species (ROS) generation, which are essential for therapeutic efficacy. This study presents a pioneering approach by combining zeolitic imidazolate framework derivatives (ZIFs) and Au NPs in a silk fibroin (SF) hydrogel for the first time. This combination not only prevents particle aggregation but also significantly enhances photothermal conversion efficiency and ROS generation capacity. The digital light processing (DLP) printability of our hydrogel allows for customized wound dressings tailored to individual patient needs, improving therapeutic efficacy. The hydrogel's effectiveness was evaluated through rigorous in vivo experiments, demonstrating enhanced antibacterial properties and accelerated wound healing. The biocompatibility of our hydrogel ensures its suitability for clinical applications, minimizing adverse reactions while promoting healing. A wound healing rate of 99.06 % represents a substantial improvement over the control groups, indicating markedly enhanced therapeutic efficacy. These findings underscore its multifunctionality in addressing infected wounds, presenting a promising strategy for facilitating the rapid healing of acute complex wounds in clinical applications.
研究领域:
生物医学工程
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材料科学
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医学
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DOI
PubMed
高影响因子
JOURNAL OF MEDICINAL CHEMISTRY
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2024
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IF 6.8
Zhiming Xing,Jiangyu Yan,Yongxiang Miao,Yawen Ruan,Haojun Yao,Youkang Zhou,Yingqun Tang,Guorui Li,Zhibin Song,Yiyuan Peng,Jing Huang
Lethal lipid peroxidation caused by reactive oxygen species occurs in different types of programmed cell death, especially in ferroptosis. Ferroptosis inducers, which serve as small-molecule probes, can provide insight into the mechanism of ferroptosis and facilitate drug discovery. The classical ferroptosis inducers indirectly lead to lipid peroxidation; thus, it is difficult to explore lipid regulation during the ferroptotic process. In this study, we designed two quinazolinone-based lipophilic probes BODIQPy-TPA and QPy-TPA, which proved to directly induce lipid peroxidation by light irradiation in vitro. The probe BODIQPy-TPA, which was mainly distributed in the endoplasmic reticulum (ER), specifically triggered ferroptosis in B16 and HepG2 cells upon light irradiation. As a comparison, the probe QPy-TPA, which was mainly distributed in lipid droplets (LDs), induced cell death by a nonferroptotic pathway. Further lipidomic analysis revealed that these two probes caused different patterns of lipid regulation and lipid peroxidation, suggesting that ferroptosis might activate distinct lipid regulation.
研究领域:
细胞生物学
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药理学
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化学生物学
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分子生物学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
·
IF 13.2
Qiaoyu Zhang,Chengcheng Chen,Fangting Liu,Zhengguo Zhang,Xiaoming Fang,Qiong Liu
The in-situ photocatalytic selective reduction of O 2 to produce H 2 O 2 is a promising green and sustainable production technique. However, it faces significant challenges due to the high reaction energy barrier of the H 2 O oxidation half-reaction, which inhibits the reaction and leads to undesirable oxidative by-products. In this study, we have the first time developed a O/Cs dual-functional carbon nitride material for the simultaneous photocatalytic reduction of O 2 to synthesize H 2 O 2 and the selective oxidation of xylose to produce xylonic acid. The CN-O/Cs material exhibits excellent photocatalytic activity for H 2 O 2 production at 820.6 μmolh −1 (41.03 mmolh -1 g −1 ), while achieving a xylose oxidation rate of 359.5 μmolh −1 to xylonic acid, surpassing most reported catalytic systems and enabling biomass upgrading. It is elucidated that the introduction of Cs atoms serves as new reduction active sites, significantly enhancing the adsorption of O 2 with the transitioning Pauling type adsorption configuration. And the Cs atoms facilitate the deprotonation capability of H 2 O to form the crucial *OOH while lowering the reaction energy barrier. The presence of oxygen atoms plays a role in redistribution of electron density, and promotes the selective oxidation of the aldehyde group at the edge of xylose. The synergistic functionalities of Cs and O atoms enable the efficient utilization of electron-hole pairs for the simultaneous synthesis of H 2 O 2 and xylonic acid. This study demonstrates that the rational design of multifunctional tandem sites materials at the atomic scale for the synergistic synthesis of H 2 O 2 and selective oxidation of biomass holds promising prospects.
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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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
En-Ze Deng,Qijie Mo,Yuying Li,Zongwen Mo,Li Zhang,Jiewei Liu
Although Z-scheme heterojunction composites have been widely studied in photocatalysis, in-depth investigation of oxygen vacancies (Ov) in the Z-scheme photocatalysts is still rare. Herein, an oxygen vacancies modified NU-1000/BiOCl-Ov composite with Z-scheme heterojunction was rationally designed and fabricated. The combination of X-ray photoelectron spectroscopy (XPS) and electron paramagnetic resonance (EPR) experiment verified the presence of oxygen vacancies, meanwhile the Z-scheme charge transfer across the heterojunction interface was confirmed in detail by the in situ -XPS, Kelvin probe force microscope (KPFM) studies, ultraviolet photoelectron spectroscopy (UPS), EPR radical capture experiment, as well as density functional theory (DFT) calculation. Importantly, compared to pristine NU-1000 and BiOCl, the optimized NU-1000/BiOCl-Ov composite displayed enhanced photocatalytic performance in the degradation of tetracycline hydrochloride (TCH) under visible light (λ ≥ 400 nm). Theoretical calculations reveal that the oxygen vacancies could induce electron redistribution, facilitating the activation of O 2 and TCH molecules, thereby promoting the photodegradation efficiency. Moreover, mechanism studies suggested that the synergistic effect of oxygen vacancies and Z-scheme heterojunction could facilitate the effective separation of photogenerated carriers. At last, the degradation routes of TCH were proposed and the toxicity of degradation intermediates was assessed. This work underlines the cooperative functions of oxygen vacancies and Z-scheme heterojunction towards improved photocatalytic performance, which offers new perspectives on the design of metal–organic frameworks (MOFs) composites for efficient photocatalysis.
研究领域:
材料科学
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环境科学
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化学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Ting Zhou,Hongjie Wang,Wenyi Dong,Tianxing Du,Xuechuan Li,Feifei Wang,Zilong Zhao
Pollution of groundwater by electron-rich refractory organic pollutants (e-ROPs) is detrimental to ecological integrity and human health. Biochar (BC)-based single-atom Fe catalysts (Fe–SACs) triggering nonradical peroxymonosulfate (PMS) process has shown great potential in addressing this problem. Nevertheless, the successful formation and precise regulation of active sites on BC remain formidable challenges. Herein, co-pyrolysis of BC derived from shrimp shells and N-containing supramolecular organic frameworks with a hexagonal cavity structure of Fe 3+ –N 3 (Fe–SOFs) was, for the first time, used to prepare an efficient and inexpensive BC-based Fe–SAC (Fe–MCA@SS). The Fe–N bond was successfully grafted from Fe–SOFs onto BC and subsequently transformed into monoatomic Fe–pyridinic N 4 . Moreover, Fe–MCA@SS successfully triggered an efficient nonradical PMS process, degrading 94.5 % of aniline (AN) within 5 min. Mediated electron transfer (MET) mechanism was primarily responsible for AN removal. MET was attributed to the following factors: the synergistic effect of the stronger chemical adsorption of PMS with an Fe atom in Fe–pyridinic N 4 active sites, the higher redox potential of [Fe–MCA@SS/PMS]*, and the value of the lowest unoccupied molecular orbital of AN being larger than the value of highest occupied molecular orbital of [Fe–MCA@SS/PMS]*. This study sheds new light on the preparation of BC-based SACs catalyst with efficient nonradical oxidation ability and an excellent feasibility to remove electron-rich organic pollutants in groundwater.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Yongjun Song,Aimin Wang,Songyu Ren,Yanyu Zhang,Ruiyan Fan,Ying Liu,Zhongguo Zhang
The utilization of hybrid electro-Fenton (EF) processes has gained considerable attention, which can combine the advantages of two or more treatment methods resulting in efficient removal of refractory pollutants from water. Here, an electro-controlled membrane coupling heterogeneous EF (EM-HEF) system was constructed for the degradation of acetaminophen (APAP) in water. In the EM-HEF system, a bifunctional ACF/CC-FeOCl-Cu cathode material was synthesized to enhance the HEF reaction, while a tubular Ti microfiltration membrane was used as both cathode and membrane. Degradation experiments indicated the EM-HEF system exhibited remarkable removal efficiency (97.0 %) towards APAP within 30 min under the conditions of flow rate at 60 mL min −1 , initial pH at 7.1, and current density at 3 mA cm −2 . Notably, the cathode materials showed low metal leaching rate and high APAP removal rate in the 10 cyclic experiments. The common inorganic anions (Cl − , HCO 3 − , HPO 4 2− , and NO 3 − ) did not inhibit the removal of APAP significantly, whereas humic acid exhibited a more pronounced inhibitory effect only at concentrations exceeding 10 mg L −1 . Quenching experiments and electron spin resonance (ESR) tests confirmed the pivotal role of hydroxyl radicals in the decomposition of APAP. Combining density functional theory (DFT) and LC-MS results, three pathways were proposed. The overall toxicity of intermediates was relieved during EM-HEF degradation of APAP. Furthermore, it also achieved good performance in the treatment of landfill leachate, with increasing BOD 5 /COD ratio from 0.11 to 0.34. This work provides an efficient strategy for the removal of refractory pollutants in water.
研究领域:
环境科学
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水处理
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化学工程
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材料科学
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计算化学
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产品关联
DOI
高影响因子
TALANTA
·
2024
·
IF 5.6
Jing Li,Shenglan Hu,Lingling Zheng,Lixin Xu,Yusheng Wu,Biyang Deng
In this study, we used meso-tetra (4-carboxyphenyl) porphyrin (TCPP) as an organic ligand to modify a lanthanide-based metal-organic framework as an electrochemiluminescence (ECL) platform to sensitively detect anti-Müllerian hormone (AMH). La-MOF amplified the ECL signal by suppressing the aggregation-caused quenching created by TCPP self-aggregation. Utilizing the reversible cycling of the mixed-valence transition metal ion (Cu + /Cu 2+ and Mo 4+ /Mo 6+ ) and the electrical conductivity of Cu 2 MoS 4 and silver nanoparticle (AgNP), Cu 2 MoS 4 –AgNP as a dual co-reaction promoter constantly generated sulfate radical anions (SO 4 •– ) and thus amplified the ECL signal. Based on this strategy, we built a sandwich-type ECL immunosensor for the sensitive detection of AMH with a linear range of 1 × 10 −4 to 50 ng/mL and a limit of detection of 24 fg/mL. This study provides a novel approach for the sensitive and selective detection of AMH, demonstrating its high potential and practical value for the sensitive detection of AMH.
研究领域:
生物医学工程
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分析化学
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免疫学
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产品关联
DOI
PubMed
高影响因子
Journal of Cleaner Production
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2024
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IF 9.7
Xueyi Zhang,Lele Qiao,Tielong Li,Haitao Wang
Every year, billions of tons of iron-rich waste are generated globally, presenting a valuable resource for synthesizing iron-based catalysts. In this study, we synthesized iron oxide-biochar (Iron Oxide@Biochar) nanocomposites by ball milling a combination of tea leaves and iron-rich waste. These nanocomposites were found to be highly efficient activators of peroxymonosulfate (PMS) for degrading tetracycline (TC). Particularly, biochar-encapsulated disposable instant hot packs (DHP/BC) achieved a TC removal efficiency of 94.7% under optimal conditions, exhibiting excellent stability and strong anti-interference capabilities. Our analysis revealed that TC degradation predominantly occurred via a non-radical pathway involving singlet oxygen ( 1 O 2 ) and electron transfer , with free radicals (·OH and SO 4 ·- ) playing a secondary role. This research not only offers an economical and efficient solution for recycling solid waste and reusing natural biochar but also introduces a sustainable and environmentally friendly method for preparing catalysts for pollutant degradation, thus achieving the dual goals of “resource recycling” and “treating waste with waste."
研究领域:
环境科学
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催化材料
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污染控制
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）