Journal of Cleaner Production
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2023
·
IF 11.1
Hao Cheng,Xinyan Li,Chao Huang,Jian Zhu,Ping Wang,Heng Cao,Chongling Feng,Dingxun Ling,Hao Liu,Min Cheng
Commercial molybdenum carbide (Mo 2 C) and ferrous iron (Fe 2+ ) were investigated for the first time to co-catalyze the activation of H 2 O 2 for the treatment of organic contaminants . Compared with traditional Fenton process, the presence of Mo 2 C decomposed hydrogen peroxide (H 2 O 2 ) more effectively and accelerated the conversion of Fe 3+ /Fe 2+ . The Rhodamine B (RhB) degradation rate constant in Mo 2 C/Fe 2+ /H 2 O 2 reached appropriately three times that in Fe 2+ /H 2 O 2 , and the co-catalytic reactivity of Mo 2 C was significantly higher than that of MoS 2 . In addition, Mo 2 C/Fe 2+ /H 2 O 2 exhibited a board effective pH range of 2.8–8.8, and four-cycle experiments confirmed the stability and reusability of Mo 2 C. The results of X-ray photoelectron spectroscopy (XPS) indicated that Mo(Ⅱ) and Mo(IV) played major roles in Fe 3+ reduction. Electron Paramagnetic Resonance analysis and quenching experiments demonstrated that hydroxyl radical (·OH), superoxide anion radical (O 2 − ) and singlet oxygen radical ( 1 O 2 ) were all involved in Mo 2 C/Fe 2+ /H 2 O 2 . Particularly, Mo 2 C/Fe 2+ /H 2 O 2 significantly enhanced the generation of ·OH and 1 O 2 in comparison to Fe 2+ /H 2 O 2 . Moreover, toxicity assessment analysis by ECOSAR suggested that the toxicity of most degradation products of RhB decreased after treatment. Overall, this study offers a promising Mo 2 C co-catalyzed Fenton process for rapid and efficient abatement of organic contaminants.
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Acta Biomaterialia
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2022
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IF 10.633
Furong Liu,Tao He,Songlin Gong,Meiling Shen,Shuang Ma,Xianzhou Huang,Lu Li,Li Wang,Qinjie Wu,Changyang Gong
Combining the internal force-driven chemodynamic therapy (CDT) and the external energy-triggered photodynamic therapy (PDT) holds great promise to achieve an advanced anticancer effect based on reactive oxygen species (ROS). However, the insufficient oxy-substrates supply in tumor microenvironment, like hydrogen peroxide (H 2 O 2 ) and oxygen (O 2 ), is the Achilles heel that greatly restricts the efficacy of this ROS-based treatment. Herein, the construction of a c opper p e roxide-based tumor pH-re s ponsive a utocatalytic nano r eactor (CESAR), via an albumin-mediated biomimetic mineralization strategy is described. The decoration of human serum albumin endows the nanoreactor good hydrophilicity and biocompatibility, which is highly desired for the metal-based materials. Upon exposure to acidic tumor microenvironment, CESAR presents a pH-triggered disintegration with Cu 2+ , H 2 O 2 and O 2 generated instantly. The generated H 2 O 2 complements the hyperoxide deficiency and initiates a localized Fenton-like reaction with the assistance of Cu 2+ for highly toxic hydroxyl radicals (•OH) production for improving CDT. The evolved O 2 gas enables hypoxia relief for enhanced Ce6-mediated PDT. This H 2 O 2 /O 2 self-supplying strategy significantly amplifies the tumor oxidative damage and gains an optimal treatment outcome, which offers a new paradigm for optimizing the tumor therapeutic options limited by oxide or hyperoxide deficiency, not only for CDT/PDT, but also other oxy-substrates involved strategies. Statement of significance The shortage of oxy-substrates in the tumor microenvironment remains a great challenge for ROS-based cancer therapy. Herein, we introduce human serum albumin as a scaffold to stabilize copper peroxide nanomaterials for constant production of H 2 O 2 and O 2 to enhance chemodynamic/photodynamic therapy. The tumor pH-triggered H 2 O 2 /O 2 production and Cu 2+ release are confirmed, assuring the strategy of a highly precise, effective way to destroy tumor without any side effects. This work lends new and exciting insights into the engineering design of autocatalytic oxy-substrates self-supply nanoreactor for overcoming the bottlenecks, like the oxy-substrates deficiency of CDT/PDT and the poor stability of metal peroxides, to achieve highly effective chemodynamic/photodynamic therapy.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
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IF 7.139
Dengyu Fu,Yanji Zhu,Lei Chen,Yue Sun,Meng Zhang,Huaiyuan Wang
Heteroatom modified catalyst applying for the two-electron oxygen reduction reaction has the potential application for efficient on-site production of H 2 O 2 . At present, state of the art catalyst synthesis is often energy-intensive and tends to destroy the original structure of heteroatoms. Based on the above considerations, Co-O, pyrrolic N structures co-modified graphite felt catalyst (Co-PDA-GF) is successfully synthesized by a simple two-step electrochemical method . Interestingly, the introduction of Co 2+ during the dopamine (DA) polymerization process changes the surface morphology of GF from a “thin-film” like to an “ant-nest” like. The cumulative H 2 O 2 concentration achieves 421 mg L −1 in 6 h test time, which is 16 times higher than that of R-GF, and the Methylene blue (MB) in-situ removal rate reaches 97.2% within 3 h. The enhanced H 2 O 2 yield of Co-PDA-GF catalyst is attributed to the increased oxygen-containing functional groups (-COOH, -C-O-C) and defect structures , and most importantly, Co-O and pyrrolic N synergistic modulation effects on local electronic modulation. This work provides new insights on DA polymerization morphology control and designing of high-efficient 2e − ORR catalyst with a low-energy method.
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Nanoscale
·
2022
·Vol. 14
·期 10
·3788-3800
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IF 8.307
Haimei Li,Yaofa Liu,Shulan Li,Silong Zhang,Biao Huang,Ran Cui,Yi Liu,Peng Jiang
Chemodynamic therapy (CDT) is a cancer treatment that converts endogenous H2O2 into hydroxyl radicals (˙OH) through Fenton reaction to destroy cancer cells. However, there are still some challenges in accelerating the Fenton reaction of CDT and improving the biodegradability of nanocatalysts. Herein, a multifunctional biomimetic BPQDs-Cu@GOD (BCG) Fenton nanocatalyst for boosting synergistically enhanced H2O2-guided and photothermal CDT of cancer is reported. Cu2+ in BCG can be reduced to Cu+ by black phosphorus quantum dots (BPQDs), triggering a Cu+-mediated Fenton-like reaction to degrade H2O2 and generate abundant ˙OH for cancer CDT. The loaded glucose oxidase (GOD) can consume the glucose in the tumor to produce abundant H2O2 for Fenton-like reaction. In addition, Cu2+ in BCG can react with GSH in tumor cells to alleviate the antioxidant capacity of tumor tissues, further improving the CDT efficacy. Furthermore, the photothermal performance of BPQDs can be enhanced by capturing Cu2+, improving the photoacoustic imaging and photothermal therapy (PTT) functions. More importantly, the enhanced photothermal performance can rapidly accelerate the Fenton-like reaction under NIR irradiation. Finally, Cu2+ can accelerate the degradation of BPQDs, which can reduce the retention of reagents. As a novel multifunctional biocompatible Fenton nanocatalyst, BCG have great potential in cancer therapy.
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INORGANIC CHEMISTRY
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2022
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IF 5.436
Hong-Mei Chai,Jia-Ling Yan,Gang-Qiang Zhang,Jia-Xing Wang,Yi-Xia Ren,Lou-Jun Gao
When a multicarboxylate aromatic ligand, 3,5-di(2′,4′-dicarboxylphenyl)benzoic acid (H5L), was employed, five structurally similar lanthanide metal–organic frameworks (Ln-MOFs), {[Pr10L6(OH)3Cl(H2O)6]·4C2H8N}n (1), {[Nd10L6(OH)4 (H2O)9]·4C2H8N}n (2), {[Gd10L6(OH)4(H2O)3]·4C2H8N}n (3), {[Ho10L6(OH)4 (H2O)3]·4C2H8N}n (4) and {[Er10L6(OH)4(H2O)6]·4C2H8N}n (5), were synthesized and characterized. Single-crystal X-ray structural analyses disclosed that all five Ln-MOFs crystallize in the trigonal R3 space group. They have three-dimensional mesoporous structure featuring the coexistence of binuclear and tetranuclear species as inorganic building units. The mesoporous structure of 3 was verified by the gas adsorption experiment of N2. Fluorescence analysis showed that 3 can selectively detect Fe3+, Cr2O72–, and H2O2; furthermore, it can be used for the electrochemical detection of trinitrophenol. With the merit of an excellent highly sensitive detection performance, 3 has unpredictable application prospects in future research fields.
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ACS Omega
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2022
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IF 4.132
Tao Chen,Yuanhong Min,Xiao Yang,Hao Gong,Xiaoying Tian,Li Liu,Yanhua Hou,Wensheng Fu
In recent years, the exploration of the nanozyme, an artificial enzyme with the structure and function of natural enzymes, has become a hot topic in this field. Although significant progress has been made, it is still a huge challenge to design nanozymes with multiple enzyme-like catalytic activities. In this work, we have successfully fabricated a colorimetric sensing platform to mimic peroxidase-like and oxidase-like activities by the CoS1.035 nanoparticles decorated N-doped carbon framework porous dodecahedrons (abbreviated to CoS1.035/N-C PDHs). And the catalytic mechanism of CoS1.035/N-C PDHs toward the peroxidase-like and oxidase-like activities is systematically explored. The results display that CoS1.035/N-C PDHs can catalyze the oxidation of the colorless substrate 3,3,′5,5′-tetramethylbenzidine (TMB) into blue oxidized TMB (ox-TMB) by disintegrating H2O2 or the physically/chemically absorbed O2 into different ROS species (·OH or O2·–) in the presence or absence of H2O2. Therefore, on the basis of the dual-enzyme mimic activities of CoS1.035/N-C PDHs, the bifunctional colorimetric sensing platform is established for H2O2 detection with a wide linear range of 0.5–120 μM and glutathione detection with a linear range of 1–60 μM, respectively. This work provides an efficient platform for dual-enzyme mimics, expanding the application prospect of Co-based chalcogenides as enzyme mimics in biosensing, medical diagnosis, and environment monitoring.
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2022
·Vol. 23
·期 7
·3799
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IF 6.208
Lulu Xiong,Yuanyuan Zhang,Shiming Wu,Feng Chen,Lingli Lei,Ling Yu,Changming Li
A facile and ingenious method to chemical etching-coordinating a metal-organic framework (MOF) followed by an annealing treatment was proposed to prepare Co3O4nanoparticles uniformly dispersed in rational porous carbon nano-boxes (Co3O4@CNBs), which was further used to detect H2O2released from living cells. The Co3O4@CNBs H2O2sensor delivers much higher sensitivity than non-etching/coordinating Co3O4, offering a limit of detection of 2.32 nM. The wide working range covers 10 nM-359 μM H2O2, while possessing good selectivity and excellent reproducibility. Moreover, this biosensor was used to successfully real-time detect H2O2released from living cells, including both healthy and tumor cells. The excellent performance holds great promise for Co3O4@CNBs’s applications in electrochemical biomimetic sensing, particularly real-time monitor H2O2released from living cells.Keywords:nano-boxes;tannic acid;Co3O4@CNBs;hydrogen peroxide sensor;electrochemical detection;living cell
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2022
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IF 4.831
Peipei Huang,Qing Chang,Guodong Jiang,Xu Wang,Haipeng Zhu,Qianqian Liu
In this article, a novel metal–organic framework, namely MIL-101(Fe II ), was firstly synthesized via a facile method. In the presence of H 2 O 2 , MIL-101(Fe II ) possesses excellent peroxidase-like activity toward the classical chromogenic substrate, N, N -Diethyl-p-phenylenediamine sulfate salt (DPD). The substitution of Fe 2+ enhances the construction of Fe(II)-oxo nodes and accelerates electrons transfer between DPD and H 2 O 2 , thereby improving the peroxidase-mimicking catalytic activity of MIL-101(Fe II ) nanoenzyme. Additionally, DPD molecules could be adsorbed readily onto the surface of the nanoparticles due to the π–π interaction. The study of Michaelis constant indicates that the MIL-101(Fe II ) exhibits a higher affinity towards DPD (0.16 mM) in contrast to horseradish peroxidase (0.78 mM). In view of the impressive catalytic performance of MIL-101(Fe II ), two reliable monitoring platforms for the rapid detection of H 2 O 2 and glucose were established with extremely low detection limits of 18.04 nM and 0.87 μM in the ranges of 40–5000 nM and 1.2–300 μM, respectively. The study of the catalytic mechanism indicates that DPD oxidation is attributed to the hydroxyl radical (·OH) produced from the decomposition of H 2 O 2 catalyzed by MIL-101(Fe II ). Furthermore, the developed sensor indicates high selectivity and stability and can be effectively appropriate for the detection of H 2 O 2 and glucose in real samples. This work not only provides a novel nanozyme with superior catalytic performance for biological analysis, but also broadens the application field of MIL-101(Fe II ) material.
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RSC Advances
·
2022
·Vol. 12
·期 32
·20838-20849
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IF 4.036
Hanzhang Ye,Yongli Ding,Tingting Liu,Jiani Li,Qi Wang,Yuhao Li,Jingjing Gu,Zhanen Zhang,Xuedong Wang
Traditional bimetallic sulfide-based nanomaterials often have a small specific surface area (SSA), low dispersion, and poor conductivity, thereby limiting their wide applications in the nanozyme-catalytic field. To address the above issues, we herein integrated NiCo2S4 with N,S-rGO to fabricate a nanocomposite (NiCo2S4@N,S-rGO), which showed a stronger peroxidase–mimetic activity than its pristine components. The SSA (155.8 m2 g−1) of NiCo2S4@N,S-rGO increased by ∼2-fold compared to NiCo2S4 with a pore size of 7–9 nm, thus providing more active sites and charge transfer channels. Based on the Michaelis–Menten equation, the affinity of this nanocomposite increased 40% and 1.1∼10.6-fold compared with NiCo2S4 with N,S-rGO, respectively, highlighting the significant enhancement of the peroxidase-like activity. The enhanced activity of this nanocomposite is derived from the joint participation of ˙OH, ˙O2−, and photogenerated holes (h+), and was dominated by h+. To sum up, N,S-codoping, rich S-vacancies, and multi-valence states for this nanocomposite facilitate electron transfer and accelerate reaction processes. The nanocomposite-based colorimetric sensor gave low detection limits for H2O2 (12 μM) and glucose (0.3 μM). In comparison with the results detected by a common glucose meter, this sensor provided the relative recoveries across the range of 97.4–101.8%, demonstrating its high accuracy. Moreover, it exhibited excellent selectivity for glucose assay with little interference from common co-existing macromolecules/ions, as well as high reusability (>6 times). Collectively, the newly developed colorimetric sensor yields a promising methodology for practical applications in H2O2 and glucose detection with advantages of highly visual resolution, simple operation, convenient use, and satisfactory sensitivity.
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Advanced Therapeutics
·
2022
·Vol. 5
·期 12
·2200108
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IF 5.003
Wen-Jie Zheng,Ze-Lei Zhou,Qi-Yan Lv,Xiaojie Song,Wen-Xing Zhang,Hui-Fang Cui
Tumor hypoxia greatly restricts photodynamic therapy (PDT) efficiency. Photothermal therapy (PTT) implemented at high temperatures induces local skin burning and surrounding tissue damage. Herein, an near-infrared (NIR)- and H 2 O 2 -double responsive heat- and O 2 -generating core–shell–shell AuNRs@MnO 2 @SiO 2 nanocarrier with Au nanorods (AuNRs) as core and MnO 2 as sandwiched nanolayer is developed to realize enhanced photodynamic/photothermal combined tumor therapy at mild-hyperthermia temperatures. Coating poly- l -lysine on AuNRs is capable of preventing AuNRs from aggregation and facilitating the on-site growth of MnO 2 . The mesoporous SiO 2 nanoshell provides large loading sites for payload indocyanine green (ICG). The MnO 2 nanolayer greatly enhances the singlet oxygen ( 1 O 2 ) generation efficiency of ICG both in testing tubes and in cancer cells. Consequently, the O 2 -enhanced PDT endows the AuNRs@MnO 2 @SiO 2 -ICG nanoparticles (NPs) dramatically stronger antitumor effect both in vitro and in vivo. Their tumor growth inhibition ratio (67.6%) is significantly higher than that of AuNRs@SiO 2 -ICG (28.5%) after one dose intratumor injection and NIR irradiation. Together with their good biosafety, the AuNRs@MnO 2 @SiO 2 -ICG is promisingly translational. The multifunctionality should provide the AuNRs@MnO 2 @SiO 2 NPs a nanocarrier platform for various therapeutic agents to modulate the tumor microenvironment and enhance tumor therapy efficiency.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Chu Dai,Xike Tian,Yulun Nie,Wei Fu,Jiatang Wang
Most researches focus on design and optimization of heterogeneous Fenton catalyst itself to drive H 2 O 2 decomposition into • OH radicals. In this study, we reported the significant impact of the interaction mode of H 2 O 2 and CuMnO 2 (namely H 2 O 2 occurrence form) on the Fenton-like performance. The interaction mode of H 2 O 2 largely exposed to Cu atom active site (CMH-L) led to a superior ofloxacin (OFX) degradation efficiency of 93% compared with H 2 O 2 middle exposed around the Cu atoms (CMH-M, 84%) and small part exposed around the Cu atoms (CMH-S, 50%). The effect of H 2 O 2 occurrence forms on catalytic activity were confirmed by analyzing their fraction and the relevant rate constant with the correlation was 98%. And the relevant interfacial reaction mechanism was detailed explored based on density functional theory calculation, a series of probe experiments and quantitative analysis of H 2 O 2 utilization efficiency and • OH generation. It revealed that Cu atom arrangement on CuMnO 2 can induce the different H 2 O 2 occurrence form, and compared with CMH-M especially CMH-S (1.486 and 1.591 Å), CMH-L has the shortest elongation of O-O bond (1.477 vs. 1.468 Å in free H 2 O 2 ) together with the smallest O-H 1 and O-H 2 (0.988, 1.022 Å), which were more likely to decomposition H 2 O 2 into • OH, while it was more likely to inefficient transformation H 2 O 2 into O 2 in CMH-S system. Thus, this work provided a new insight for improving the heterogeneous Fenton catalytic performance via altering the interaction mode of H 2 O 2 and catalyst, which should be the fundamental reason for efficient H 2 O 2 activation into O 2 or • OH.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Bingliang Zhang,Zhuoyao Fang,Shu Wang,Xifeng Shi,Bo Guo,Jie Gao,Dandan Wang,Wansong Zong
Ozonation and ultraviolet-based advanced oxidation processes (UV-AOPs) play important roles in advanced treatment of municipal wastewater for water reuse . Bromide is widely present in wastewater at different concentration levels (ranging from μg/L to mg/L). However, the effect of bromide on molecular transformation of dissolved effluent organic matter (dEfOM) in real wastewater during ozonation and UV-AOPs treatments still remains unclear. Herein, Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) was utilized to characterize the overall molecular transformation of dEfOM and the formation of unknown halogenated byproducts (X-BPs) in ozonation, UV/H 2 O 2 , UV/persulfate (UV/PS), and UV/chlorine (UV/Cl) processes in the presence of additional bromide. Compared with the same oxidation processes without additional bromide, the degree of dEfOM oxygenation had some extent decrement with the effect of bromide. A slightly increment of the number of unknown brominated byproducts (Br-BPs) was observed during ozonation, UV/H 2 O 2 , and UV/PS treatments in the presence of additional bromide, and the largest increment of these compounds was found in UV/Cl process. A total of 82 chlorinated byproducts (Cl-BPs) and 183 Br-BPs were detected in all oxidation processes with the effect of bromide, and the number of Br-BPs was significantly higher than that of Cl-BPs. Based on mass difference analysis, 69 pairs of possible precursors/Br-BPs were identified. In addition, the additional bromide did not remarkably increase the concentrations of trihalomethanes (THMs) and haloacetic acids (HAAs) in ozonation, UV/H 2 O 2 , and UV/PS treatments, while the production of THMs and HAAs significantly decreased by 68.06% and 54.55%, respectively, during UV/Cl treatment. The calculated cytotoxicity increased to some extent for each treatment, especially for UV/Cl treatment, and the compound with largest contribution to cytotoxicity was monobromoacetic acid. This study provides new insights into the formation and transformation of X-BPs during advanced treatment of real wastewater with the effect of bromide.
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