JOURNAL OF NANOBIOTECHNOLOGY
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2022
·Vol. 20
·期 1
·1-19
·
IF 9.429
Jia Tao,Li Dan,Du Jiarui,Fang Xikui,Gerasimov Valeriy,Ågren Hans,Chen Guanying
Nanozymes are promising for precise cancer treatment, but are typically limited in terms of the low catalytic efficiency and the complexity in tumor microenvironment (TME). Herein, we describe a bimodal type of AgPd plasmonic blackbody (AgPd PB) nanozyme of compact sizes (< 30 nm), which presents not only boosted enzyme efficacy but also efficient photothermal therapy (PTT) for synergized therapy through tissue-penetrating light in the second biological window (1000–1700 nm). The synthesized hyperbranched AgPd PB nanozymes possess intense and broadband localized surface plasmonic resonance absorption of 400–1300 nm, entailing prominent photothermal efficiency (η = 45.1% at 1064 nm) for PTT. Importantly, PTT was found to significantly boost the nanozyme efficacy of both catalase (CAT) and peroxidase (POD) processes, which correspondingly decompose H2O2 to into O2 to relieve tumor hypoxia, and activate H2O2 to generate oxidative •OH radical. While the generated •OH was found to be able to minimize heat shock proteins (HSPs), which plays a vital role to counterbalance PTT effect both in vitro and in vivo. As compared to control ground without treatment, the synergized nanozyme and PTT activities resulted in about 7-fold reduction of tumor volume, thus elevating the survival rate from 0 to 80% at 30 days posttreatment. Besides the synergistic therapy, the AgPd PB nanozyme were shown to own fluorescence, computed tomography (CT), and photoacoustic (PA) imaging abilities, thus having implications for uses in imaging-guided precise cancer therapy. This study provides a paradigm of TME responsive theranostics under NIR-II light irradiation.Graphical Abstract
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高影响因子
WATER RESEARCH
·
2022
·
IF 13.4
Wenxiao Zheng,Yingkai Chen,Hengyi Fu,Zhang Yan,Zhenchao Lei,Weijian Duan,Chunhua Feng
The generation of chlorinated byproducts during the electrochemical oxidation (EO) of Cl − -laden wastewater is a significant concern. We aim to propose a concept of converting reactive species (e.g., reactive chlorines and HO • resulting from electrolysis) into 1 O 2 via the addition of H 2 O 2 , which substantially alleviates chlorinated organic formation. When phenol was used as a model organic compound, the results showed that the H 2 O 2 -involving EO system outperformed the H 2 O 2 -absent system in terms of higher rate constants (5.95 × 10 −2 min −1 vs. 2.97 × 10 −2 min −1 ) and a much lower accumulation of total organic chlorinated products (1.42 mg L −1 vs. 8.18 mg L −1 ) during a 60 min operation. The rate constants of disappearance of a variety of phenolic compounds were positively correlated with the Hammett constants ( σ ), suggesting that the reactive species preferred oxidizing phenols with electron-rich groups. After the identification of 1 O 2 that was abundant in the bulk solution with the use of electron paramagnetic resonance and computational kinetic simulation, the routes of 1 O 2 generation were revealed. Despite the consensus as to the contribution of reaction between H 2 O 2 and ClO − to 1 O 2 formation, we conclude that the predominant pathway is through H 2 O 2 reaction with electrogenerated HO • or chlorine radicals (Cl • and Cl 2 • − ) to produce O 2 • − , followed by self-combination. Density functional theory calculations theoretically showed the difficulty in forming chlorinated byproducts for the 1 O 2 -initiated phenol oxidation in the presence of Cl − , which, by contrast, easily occurred for the Cl • -or HO • -initiated phenol reaction. The experiments run with real coking wastewater containing high-concentration phenols further demonstrated the superiority of the H 2 O 2 -involving EO system. The findings imply that this unique method for treating Cl − -laden organic wastewater is expected to be widely adopted for generalizing EO technology for environmental applications.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Kai Feng,Jiang Gong,Jinping Qu,Ran Niu
Micro/nanomotors have emerged as a vibrant research topic in biomedical and environmental fields due to their attractive self-propulsion as well as small-scale functionalities. However, single actuated micro/nanomotors are not adaptive in facing intricate natural and industrial environments. Herein, we propose a new dual-mode-driven micromotor based on foam-like carbon nitride (f-C3N4) with precipitated Fe3O4 nanoparticles, namely, Fe3O4/f-C3N4, powered by chemical/magnetic stimuli for rapid reduction of organic pollutants. The Fe3O4/f-C3N4 motor composed of a three-dimensional (3D) porous “foam-like” structure and precipitated Fe3O4 nanoparticles (ca. 50 nm) not only exhibits efficient photocatalytic performance under visible light but also shows versatile and programmable motion behavior under the control of external magnetic fields. The aggregation of the micromotor under an external rotating magnetic field further enhances the catalytic activity by the increased local catalyst concentration. Furthermore, the magnetic property endows the micromotor with easy recyclability. This study provides a novel dual-mode-driven micromotor for antibiotics removal with magnetic field and light-enhanced performance in industrial wastewater treatment at a low cost.
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Environmental Science-Nano
·
2022
·Vol. 9
·期 11
·4162-4176
·
IF 9.473
Qiuxia Liu,Yuelong Wang,Meicheng Wen,Yunlong Guo,Yupeng Wei,Guiying Li,Taicheng An
Formaldehyde has strong carcinogenic and cancer-promoting effects, and its removal from indoor air is still challenging. Transition metal oxides such as cobalt(II,III) oxide (Co3O4) are potential catalysts to eliminate formaldehyde. However, the inherent low activity of Co3O4 at room temperature has greatly limited its utilization for indoor air purification. In this work, an extremely facile and mild method was designed to prepare a Au@Co3O4 core–shell nanocomposite catalyst, and its catalytic and photocatalytic activities for formaldehyde oxidation were determined both under dark conditions and visible-light irradiation. This material exhibited not only high catalytic formaldehyde oxidation efficiency in the absence of light but also significantly promoted photocatalytic formaldehyde oxidation activity under visible-light irradiation. Electron paramagnetic resonance and in situ diffuse reflectance infrared Fourier transform spectroscopy were applied to identify the reactive oxygen species and the produced degradation intermediates which adsorbed onto the surface of the catalyst during the oxidation process. It was found that the enhanced catalytic activity of the Au@Co3O4 nanocomposite catalyst under visible-light irradiation was mainly attributed to the promotion of oxygen and formaldehyde activation by the photogenerated carriers, facilitating the formation of dioxymethylene and thereby accelerating the key step of the generation of formic acid and carbonate species. This fundamental study provides evidence for a catalytic mechanism of the photocatalytic degradation of formaldehyde and a basis for the rational design of catalysts that efficiently eliminate indoor formaldehyde through full use of visible light.
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Journal of Cleaner Production
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2022
·
IF 11.072
Mingjun Xu,Qian Zhang,Ziqi Zhu,Yuwei Xue,Ting Zhang,Junming Hong
Prussian blue analogs (PBAs) have been widely explored as catalyst for peroxymonosulfate (PMS) activation. However, the drawbacks of poor electron transfer ability and degradation performance of PBAs hinder their practical application. In this study, oxygen vacancy (OV)-rich Mn-Fe PBA was regulated through phosphoric acid and ammonia water chemical etching to overcome these drawbacks. Experimental and theoretical investigations indicated that the regulation of OVs was favorable for more Fe 2+ and Mn 3+ active sites exposure and higher specific surface area to facilitate PMS activation. Sulfate radical (SO 4 •− ), hydroxyl radical (HO•), and single oxygen ( 1 O 2 ) were verified as main reactive species for PMS activation during catalytic reaction . Density functional theory calculation results showed that the OV-rich NOE-PC-300 had the highest pollutants degradation capability, with complete degradation of bisphenol A (BPA) and acetaminophen (APAP) within 40 min. Through regulation of OVs by chemical etching, highlighted adsorption ability and elongated O–O bond of PMS were obtained. This research showed that NOE-PC-300 is an efficient and harmless catalyst for activating PMS, and it has immense application potential in practical wastewater treatment .
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CHEMICAL PHYSICS LETTERS
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2022
·
IF 2.719
Jing Kong,Jingui Zhang,Ming Shen,Sufen Zhang,Peipei Shen,Chuanli Ren
Bacterial infection is a major cause of life-threatening infections. Zinc oxide nanoparticles (nano-ZnO) are an inorganic antimicrobial material with non-toxicity and low antimicrobial efficiency. To improve its antimicrobial activity, a series of manganese(II) oxide/ZnO nanocomposites were designed and prepared via a chemical precipitation method. After being characterized via EDS, XRD, SEM, TEM, and HRTEM, the obtained nanocomposites were proved to be successful with no impurities and exhibited smaller particle sizes. It showed improved photocatalytic activity and antibacterial activity under visible light. The MnO/ZnO-2.5% nanocomposite showed 92.3% inhibition against E. coli . MnO/ZnO nanocomposites can kill bacteria by generating reactive oxygen species.
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Journal of Environmental Sciences
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2022
·
IF 6.796
Wenxia Wang,Zhen Li,Kailin Wu,Guodong Dai,Qingping Chen,Lihua Zhou,Junxia Zheng,Liang Ma,Guiying Li,Wanjun Wang,Taicheng An
Rational design and synthesis of highly efficient and robust photocatalysts with positive exciton splitting and interfacial charge transfer for environmental applications is critical. Herein, aiming at overcoming the common shortcomings of traditional photocatalysts such as weak photoresponsivity, rapid combination of photo-generated carriers and unstable structure, a novel Ag-bridged dual Z-scheme g-C 3 N 4 /BiOI/AgI plasmonic heterojunction was successfully synthesized using a facile method. Results showed that Ag-AgI nanoparticles and three-dimensional (3D) BiOI microspheres were decorated highly uniformly on the 3D porous g-C 3 N 4 nanosheet, resulting in a higher specific surface area and abundant active sites. The optimized 3D porous dual Z-scheme g-C 3 N 4 /BiOI/Ag-AgI manifested exceptional photocatalytic degradation efficiency of tetracycline (TC) in water with approximately 91.8% degradation efficiency within 165 min, outperforming majority of the reported g-C 3 N 4 -based photocatalysts. Moreover, g-C 3 N 4 /BiOI/Ag-AgI exhibited good stability in terms of activity and structure. In-depth radical scavenging and electron paramagnetic resonance (EPR) analyses confirmed the relative contributions of various scavengers. Mechanism analysis indicated that the improved photocatalytic performance and stability were ascribed to the highly ordered 3D porous framework, fast electron transfer of dual Z-scheme heterojunction, desirable photocatalytic performance of BiOI/AgI and synergistic effect of Ag plasmas. Therefore, the 3D porous Z-scheme g-C 3 N 4 /BiOI/Ag-AgI heterojunction had a good prospect for applications in water remediation. The current work provides new insight and useful guidance for designing novel structural photocatalysts for environment-related applications.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
·
IF 14.224
Yuchen Zhang,Peng Zhou,Rongfu Huang,Chenying Zhou,Yang Liu,Heng Zhang,Xiaowei Huo,Jian Zhao,Zhaokun Xiong,Bo Lai
The regeneration of Fe(II) is the rate-limiting step in the Fenton/Fenton-like chain reactions that seriously hinder their scientific progress towards practical application. In this study, we proposed iron boride (FeB) for the first time as a new material to sustainably decompose H 2 O 2 to generate hydroxyl radicals , which can non-selectively degrade a wide array of refractory organic pollutants . Fe(II) can be steadily released by the stepwise oxidation of FeB to stimulate Fenton reaction, meanwhile, B-B bonds as electron donors on the surface of FeB effectively promote the regeneration of Fe(II) from Fe(III) species and significantly accelerate the production of hydroxyl radicals. The low generation of toxic by-products and the high utilization rate of iron species validly avoid the secondary organic/metal pollution in the FeB/H 2 O 2 system. Therefore, FeB mediated Fenton oxidation provides a novel strategy to realize a green and long-lasting environmental remediation.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Mengxiang Ye,Chao Zhang,Zhenzhen Liu,Huaimeng Li,Zhen Fu,Haimin Zhang,Guozhong Wang,Yunxia Zhang
Extensive utilization and excessive accumulation of bisphenol A (BPA) has posed a serious threat to the whole ecosystem, necessitating the rational design of metal-based catalysts capable of complete mineralization of BPA via electrochemical oxidation. Considering the shortage of metals resources and ever-increasing generation of electronic waste (e-waste), converting e-waste into high-performance catalysts is highly expected to offer an economical and feasible means to achieve the degradation of BPA. To this end, CuAu bimetallic catalysts are in situ electro-codeposited on the carbon cloth (CC) support with the waste central processing unit (CPU) leachate as electrolyte. Significantly, the recovered CuAu/CC composites can be directly applied as an efficient electrocatalyst for the decontamination of BPA via the electro-Fenton process. The electrocatalytic activities of the fabricated CuAu/CC electrodes can be regulated by tuning the reduction potentials during electro-deposition process. Under the optimized operational conditions, 99.5 % of BPA (50 mg/L) is removed within 120 min at a constant cathodic potential of −1.0 V (vs Ag/AgCl) in the CuAu/CC-mediated electro-Fenton system, accompanied by 64.2 % of total organic carbon (TOC) removal, highlighting a satisfactory performance of the BPA electrochemical oxidation. In addition, the proposed CuAu/CC electrode material can be facilely regenerated and reused for at least ten cycles without significant decline in BPA removal efficiency. Our work offers valuable guidance for upcycling of bimetallic alloy catalysts from e-waste and further application in electrochemical decontamination of organic pollutants, achieving the innovative target of “using waste to treat waste.”
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ANALYST
·
2022
·Vol. 147
·期 23
·5355-5362
·
IF 5.227
Yi Xia,Jiaxin Zhou,Yanying Liu,Yutong Liu,Ke Huang,Huimin Yu,Xue Jiang,Xiaoli Xiong
Due to their high catalytic activity, stability and low cost, nanozymes with oxidase-like activity have attracted widespread interest in the fields of analytical detection and colorimetric sensing. To further promote the catalytic activity and the sensitivity of dopamine (DA) sensing, herein, a mixed valence Ce-MOF (MVCM) with enhanced oxidase-like activity was synthesized by the dielectric barrier discharge (DBD) microplasma method. Compared with hydrothermal synthesis, the prepared MVCM synthesized using a microplasma showed a higher catalytic activity, which benefits from a low Ce3+/Ce4+ ratio. Due to the spontaneous redox properties of Ce3+/Ce4+ in a MVCM, the MVCM-based colorimetric sensing of dopamine was established and showed a limit of detection of 0.74 μM over a linear range of 5–100 μM with high selectivity and stability and has been applied for the detection of dopamine in sweat. The proposed study provides an effective synthesis method for nanozymes with enhanced activity and shows great promise in widespread analytical and sensing applications.
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MICROCHIMICA ACTA
·
2022
·Vol. 189
·期 11
·1-15
·
IF 6.408
Qin Dongmiao,Meng Shuo,Wu Yusheng,Luo Zhi,Deng Biyang
An efficient electrochemiluminescence resonance energy transfer (ECL-RET) method is proposed which combines the luminescent materials of tris(4,4′-dicarboxylicacid-2,2′-bipyridyl) ruthenium(II) (energy donor) and tin dioxide and tin disulfide quantum dots (SnO 2 /SnS 2 QDs) (energy acceptor) into the isoreticular metal − organic framework-3 (IRMOF-3) material to form a composite. In this mode, the distance between the energy donor and the acceptor was greatly shortened, reducing the energy loss, and thereby effectively improving RET efficiency and further significantly improving the ECL signal. The obtained composite (SnO 2 /SnS 2 QDs-Ru@IRMOF-3) was combined with sandwich immunoreaction to construct an ECL immunosensor for the sensitive detection of procalcitonin (PCT). Under the optimized experimental conditions with a working potential of − 1.48 V (vs Ag/AgCl), the proposed PCT biosensor exhibited a linear concentration range of 1 × 10 −4 –200 ng mL −1 , with a detection limit of 0.029 pg mL −1 ( S / N = 3). The biosensor was used to detect PCT in actual samples. The biosensor has broad application prospects in biological analysis and clinical diagnosis due to its high sensitivity, good selectivity, and good stability. Graphical abstract
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Xinyi Zhang,Weibao Liu,Yuerong Zhou,Yunhe Li,Ying Yang,Jianfeng Gou,Jiangwei Shang,Xiuwen Cheng
In order to further expand the practical applicability of nano photo-activators, a low-toxicity bismuth ferrite mixture (BFO) combined with MnO 2 were used to construct nano-catalyst@nickel foam (NF) composite material. A variety of characterization methods were applied to determine the physical, chemical and photoelectrochemical properties of BFO/MnO 2 @NF. Subsequently, the performance of BFO/MnO 2 @NF/PMS/Light degradation system was evaluated through the enrofloxacin (ENR) removal experiment. And 87.5% of ENR could achieve removal with 4 cm 2 of BFO/MnO 2 (3:1)@NF and 0.6 g L −1 of peroxymonosulfate (PMS) at the pH of 6.86 in the coupled system. In addition, during the ENR degradation process, the leaching percentages of Bi, Fe, and Mn ions in the BFO/MnO 2 nano powder and BFO/MnO 2 @ NF were 0.041%, 0.29%, 0.12% and 0.035%, 0.068%, 0.084% (0.035% of Ni dissolution), respectively. It could be seen that the leaching concentration of metal ions during the reaction of the nickel foam-supported composite material was much lower than that of the corresponding nano-catalysts powder. Furthermore, the coupled system maintained excellent catalytic performance even after 8 running cycles. Thus, the BFO/MnO 2 @NF was easy to recover from the system and met the needs of practical applications, which would provide more opportunities for the design of nano-catalysts and practical applications in wastewater treatment processes.
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