ANALYTICAL CHEMISTRY
·
2025
·
IF 6.7
Fei Hu,Kaihui Liu,Yunyun Zhang,Shuhao Zhao,Tianyi Zhang,Cuiping Yao,Xing Lv,Jing Wang,Xiaolong Liu,Niancai Peng
Infectious diseases, especially respiratory infections, have been significant threats to human health. Therefore, it is essential to develop rapid, portable, and highly sensitive diagnostic methods for their control. Herein, a short-time preamplified, one-pot clustered regularly interspaced short palindromic repeats (CRISPR) nucleic acid detection method (SPOC) is developed by combining the rapid recombinase polymerase amplification (RPA) with CRISPR-Cas12a to reduce the mutual interference and achieve facile and rapid molecular diagnosis. SPOC can reduce the detection time and stably detect up to 1 copy/μL of severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) RNA without affecting the detection sensitivity. A highly sensitive one-pot assay integrated with reverse transcription RPA is achieved by wrapping paraffin with a specific melting point on the lyophilized CRISPR reagent surface. A self-heating pack is designed based on thermodynamic principles to melt the paraffin and release CRISPR reagents, enabling low-cost and time-saving detection. Notably, the designed system, coupled with RNA extraction-free technology, can achieve “sample-in-answer-out” detection of the SARS-CoV-2 Orf1ab gene within 22 min using smartphone imaging. The developed assay is validated on 12 clinical samples, and the results 100% correlate with real-time polymerase chain reaction. SPOC is time-saving, is easy to operate, and can eliminate centrifugal and complex hardware devices, satisfying the demand for point-of-care diagnostics in resource-constrained settings.
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ACS Nano
·
2024
·
IF 15.8
Xianghua Wu,Lei Zhang,Yifan Tong,Long Ren,Huiru Guo,Yang Miao,Xun Xu,Yuan Ji,Fangzhi Mou,Yu Cheng,Jianguo Guan
Magnetic liquid-bodied microrobots (MRs) possess nearly infinite shape adaptivity. However, they currently confront the risk of structure instability/crushes during shape-morphing in tiny biological environments. This article reports that magnetic liquid metal (LM) MRs (LMMRs) show high structure stability and robust magnetic maneuverability. In this protocol, Fe nanoparticles are encapsulated inside less-than-10-μm LM microdroplets by establishing interfacial chemical potential barriers, yielding LMMRs. Their robust magnetic maneuverability originates from the magnetically controlled assembly of Fe nanoparticles inside LM and distinct liquid–solid interaction. With the self-adaptive shape-recovering capabilities even after 50% deformation, LMMRs can implement vertical climbing over walls up to 400% of its body length and traverse channels with the size of its two-thirds. The in vitro and in vivo experiments have both verified the effective magneto-mechanical stimulation of LMMRs upon neurons after their shape-adaptive crossing the blood–brain barrier under a driven magnetic field. Our work provides a promising strategy for wireless therapies with MRs by safely and effectively overcoming biological barriers.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Yuhang Zhang,Hao Zhang,Nuanqin Zhang,Biao Zhou,Falong Jia,Lizhi Zhang,Zhihui Ai,Xiao Liu
Cadmium (Cd) contamination is highly toxic to human health, and the complexed Cd in wastewater is tricky to remove owing to its stable chelating structure. In this study, industrial zero-valent iron (ZVI) was modified by ball-milling with tiny formic acid (FA), and the as-prepared sample (FA-ZVI bm ) was attempted in the treatment of Cd II -ethylenediaminetetraacetic acid (Cd II -EDTA). Little FA addition to ball-milling could dramatically improve the performance of FA-ZVI bm towards Cd II -EDTA elimination and raise the elimination rate constant by more than 200 times. Results ascertained that the (HCOO) 2 Fe II shell formed on FA-ZVI bm promoted Cd II -EDTA decomplexation and activation of dissolved O 2 to reactive oxygen species (ROS) for oxidative degradation of EDTA ligands. Cd II -EDTA was instantly decomplexation by Fe 3+ replacement, and the decomplexed Cd 2+ was rapidly captured by FA-ZVI bm . At the same time, the EDTA ligands underwent oxidative degradation, avoiding the re-chelation ecological hazard. Interestingly, we found that replacement decomplexation has a synergistic mechanism for activating dissolved O 2 to ROS , facilitating oxidative destruction of EDTA ligands. Furthermore, the FA-ZVI bm fixed-bed reactor could remediate Cd II -EDTA contaminated environmental water one-stop, and the effluent stably meets the emission standards. This study demonstrated that FA-ZVI bm could be a viable approach for Cd II -EDTA decontamination and clarified the remediation mechanism.
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Journal of Cleaner Production
·
2024
·
IF 9.7
Linfang Li,Qing Lin,Xiaobin Liao,Tianze Liu,Huan Qi,Qingsong Li,Menglan Gao,Jing Zou,Zhenming Zhou,Mingzhi Huang,Zhimin Yang
The widespread amines have been found to generate carcinogenic nitro-dimethylamine (NDMA) during ozonation, it's urgent to search effective methods to control its formation. This work investigated the performance and mechanisms of bimetallic organic framework (MIL-100(Fe-Mn)) on reducing NDMA production during ozonation of daminozide (DMNZD). The results demonstrated that NDMA concentration raised from 27.6 to 248.4 μg/L when ozone dosages enhanced from 0.5 to 4 mg/L; while just slightly increased from 0.9 to 3.7 μg/L when MIL-100 (Fe-Mn) was added, with a reduction rate up to 98.5 %. When catalyst dosages increased from 0 to 200 mg/L, NDMA reduction rates enhanced from 54.5 to 97.4%. Moreover, neutral conditions facilitated the exploitation of MIL-100(Fe-Mn) during ozonation. Water bodies containing high concentrations of CO 3 2− , HA, and Br − should be avoided to prevent high NDMA risk. MIL-100(Fe-Mn) enhanced the transformation of ozone molecular (O 3 ) to hydroxyl radical (·OH) other than superoxide radicals (·O 2 − ) and singlet oxygen ( 1 O 2 ). EPR and scavengers quenching experiments verified that ·OH played important roles in NDMA reduction. Except ·OH, hydrogen radicals (·H) were detected in catalyzed ozonation system for the first time. The results would provide new insights for NDMA risks control during ozonation.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2024
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IF 8.2
Zhenyu Zhao,Zhengwei Zhou,Xiaomeng Zhang,Chengsi Hou,Deli Wu
Pyrite-based Fenton-like processes have been extensively studied for wastewater decontamination; however, most relevant studies placed excessive emphasis on the homogeneous Fenton reaction mediated by aqueous Fe 2+ , resulting in the proposed technologies facing issues such as additional acid requirements for pH adjustment and excessive iron sludge production. Herein, through in situ shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS), custom dual-chamber reactor experiments, and a series of control experiments, significant hydroxyl radical generation was identified during the pyrite/H 2 O 2 process, while the dominant reactive iron species was verified to the structural Fe sites on the pyrite surface, rather than structural Fe(II) in secondary iron minerals and surface adsorbed Fe 2+ . Consequently, even with significant suppression of the homogeneous Fenton pathway, the pyrite/H 2 O 2 process exhibited significant degradation efficiency for sulfamethoxazole (SMX) at pH 4. Moreover, the pyrite/H 2 O 2 process was found to selectively remove 50 μM of pollutants with high affinity for pyrite (bisphenol A, carbamazepine, nitrobenzene, and SMX), even in the presence of 50–100 mM methanol. Compared to the typical iron-based reductive catalyst (zero-valent iron, ZVI), pyrite mediated a Fenton process with greater potential for practical applications at pH 4, achieving a 43.75-fold reduction in iron sludge production and almost doubling the H 2 O 2 utilization efficiency. Additionally, in contrast to ZVI, minimal iron oxide formed on the pyrite surface during the oxidation process. Thus, after seven cycles of degradation experiments, the decontamination efficiency of the pyrite/H 2 O 2 process remained stable. These findings are crucial for understanding the complex environmental behavior of pyrite in both natural and engineering processes and provide a new perspective for the efficient utilization of pyrite resources as well.
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RSC Advances
·
2024
·Vol. 14
·期 8
·5417-5424
·
IF 3.9
Jie Yi,Yajing Yang,Xi-ming Song,Yuxuan Zhang
Azobenzene-containing poly(aryl ether)s are a potential type of photoinduced deformable high-performance polymer. However, research on photoinduced deformation of azobenzene-containing poly(aryl ether)s focuses mainly on poly(aryl ether)s containing azobenzene groups in the main chain. In this paper, the photoinduced deformation of poly(aryl ether)s containing azobenzene groups in the side chain was studied for the first time. Two novel poly(aryl ether)s containing azobenzene groups in the side chain were synthesized, and their photoinduced isomerization behavior and photoinduced deformation behavior were studied. It could be seen that the match of the excitation luminescence to the maximum absorption peak of the azobenzene groups was more compatible, and the photoinduced motion of the polymers was faster. In addition, poly(aryl ether)s containing azobenzene groups in the side chain showed highly stable photoinduced deformation. The results of this work will be helpful for designing polymers which could be controlled by lasers of different wavelengths.
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DALTON TRANSACTIONS
·
2025
·Vol. 54
·期 8
·3467-3477
·
IF 3.3
Wenhui Hu,Zhongxin Song,Lingna Sun,Lei Zhang,Qianling Zhang,Xiangzhong Ren,Yongliang Li
Efficient separation of photogenerated charge carriers is essential for maximizing the photocatalytic efficiency of semiconductor materials in oxygen evolution reactions (OER). This study presents a novel trimetallic photocatalyst, MIL-100(Fe)/TiO2/CoOx, synthesized through a facile microwave-assisted hydrothermal method followed by atomic layer deposition (ALD). The porous MIL-100(Fe) serves as a support for the sequential deposition of TiO2 and CoOx layers via ALD, which enhances electron–hole pair separation and minimizes their recombination. Characterization using transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) confirms the uniform deposition of TiO2 and CoOx layers on the MIL-100(Fe) surface. The optimized photocatalyst, processed with 20 deposition cycles of Co, exhibits exceptional photocatalytic OER performance, with an oxygen evolution rate of 558.3 μmol g−1 h−1. This enhancement in activity is attributed to the synergistic interaction between the spatially separated TiO2 and CoOx cocatalysts, which facilitates efficient charge transfer and increases the number of active sites. These findings highlight the potential of ALD-fabricated heterostructures in the development of advanced photocatalysts for sustainable energy production.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Cong Wan,Jianwen Zhang,Honglei Zhang,Min Liu,Yiming Li,Zijun Yan,Chengheng Pang,Tao Wu
The catalytic reduction of CO₂ into valuable chemicals and fuels is a promising strategy for mitigating global carbon emissions. This study explores the synergistic co-reduction of CO₂ and H₂O using nanoscale zero-valent iron (NZVI) as a dual-function catalyst. Under light irradiation at 300 °C, the CO₂ reduction rate increased by more than 10-fold compared to dark conditions, demonstrating significant photothermal synergy. The study reveals that NZVI undergoes a phase transformation, where Fe₃O₄ functions as a photocatalyst while Fe 0 serves as an electron donor, enabling a unique dual-functionality that facilitates efficient electron transfer. The addition of 10 vol% H₂ stabilizes the reaction, leading to a higher and more consistent CO yield. When investigating the simultaneous reduction of CO₂ and H₂O, we discovered competitive adsorption and reaction pathways that significantly influence product distribution. In-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and density functional theory (DFT) calculations revealed three distinct mechanistic pathways for CO₂ conversion: direct C O bond cleavage, a carboxylate-mediated pathway and bicarbonate-mediated pathway, with the carboxylate and bicarbonate pathways being uniquely promoted by H and OH from H₂O dissociation. The addition of H₂O into the CO₂ and H₂ reaction significantly enhanced CH₄ generation due to the extra H source from H₂O dissociation. These findings offer valuable insights into the competitive mechanistic pathways of CO₂-H₂O co-reduction and contribute to the design of more efficient iron-based catalysts for sustainable CO₂ conversion and water splitting in energy and environmental applications.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Shichao Cai,Jiawei Zhao,Yurou Tan,Zhongkuan Wu,Bo Chen,Feng He
In this study, we synthesized microscale sulfidated zerovalent iron (S-mZVI) with controllable mackinawite (FeS) content up to nearly 100 wt % and investigated the roles of FeS and Fe0 for arsenite (As(III)) sequestration under aerobic conditions. Batch experiments show that FeS and Fe0 contents determine the kinetics and longevity of As removal by S-mZVI, respectively. The Fe0/FeS galvanic cell accelerates the consumption of Fe0 by dissolved oxygen (DO) while preserving FeS to preferentially remove As as sulfide, which is protected from oxidation by Fe0. In column studies, mZVI and S0 were mixed in sand to form S-mZVI in situ. Results of sequential extraction of reacted S-mZVI particles from different column zones and run stages further indicate that As formed as sulfide by S-mZVI, which was then oxidized by DO after Fe0 depletion to form As-iron (hydr)oxides. X-ray absorption near-edge structure characterization confirmed that As sulfide is mainly in the form of realgar (As4S4). S-mZVI (2 wt % of column sand) reduces total As from 2 mg/L to 10 μg/L, up to 300 bed volumes, with a residence time of 70 min. In situ synthesis and cost advantages make S-mZVI a promising method to address As contamination issues worldwide.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
·
IF 10.8
Lihang Ma,Yi-bo Hu,Shuhan Li,Ting Du,Xinran Xiong,Yuanhuan Wu,Xiao-yan Li,Ming-Lai Fu,Baoling Yuan
Nanoscale zerovalent iron synthesized using borohydride (B-NZVI) has been widely applied in environmental remediation in recent decades. However, the contribution of boron in enhancing the inherent reactivity of B-NZVI and its effectiveness in removing hexavalent chromium [Cr(VI)] have not been well recognized and quantified. To the best of our knowledge, herein, a core–shell structure of B-NZVI featuring an Fe–B alloy shell beneath the iron oxide shell is demonstrated for the first time. Alloyed boron can reduce H+, contributing to more than 35.6% of H2 generation during acid digestion of B-NZVIs. In addition, alloyed B provides electrons for Fe3+ reduction during Cr(VI) removal, preventing in situ passivation of the reactive particle surface. Meanwhile, the amorphous oxide shell of B-NZVI exhibits an increased defect density, promoting the release of Fe2+ outside the shell to reduce Cr(VI), forming layer-structured precipitates and intense Fe–O bonds. Consequently, the surface-area-normalized capacity and surface reaction rate of B-NZVI are 6.5 and 6.9 times higher than those of crystalline NZVI, respectively. This study reveals the importance of alloyed B in Cr(VI) removal using B-NZVI and presents a comprehensive approach for investigating electron pathways and mechanisms involved in B-NZVIs for contaminant removal.
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WATER RESEARCH
·
2024
·
IF 11.4
Sheng Deng,Yu Yang,Xu Han,Qiyuan Liu,Mingxiao Li,Jing Su,Yonghai Jiang,Beidou Xi,YuHui Liu
Numerous investigations have illuminated the profound impact of phosphate on the adsorption of uranium, however, the effect of phosphate-mediated surface modification on the reactivity of zero-valent iron (ZVI) remained enigmatic. In this study, a phosphate-modified ZVI (P-ZVI bm ) was prepared with a facile ball milling strategy, and compared with ZVI bm , the U(VI) removal amount (435.2 mg/g) and efficiency (3.52×10 −3 g·mg −1 ·min −1 ) of P-ZVI bm were disclosed nearly 2.0 and 54 times larger than those of ZVI bm respectively. The identification of products revealed that the adsorption mechanism dominated the removal process for ZVI bm , while the reactive modified layer strengthened both the adsorption pattern and reduction performance on P-ZVI bm . DFT calculation result demonstrated that the binding configuration shifted from bidentate binuclear to multidentate configuration, further shortening the Fe-U atomic distance. More importantly, the electron transferred is more accessible through the surface phosphate layer, and selectively donated to U(VI), accounting for the elevated reduction performance of P-ZVI bm . This investigation explicitly underscores the critical role of ZVI's surface microenvironment in the domain of radioactive metal ion mitigation and introduces a novel methodology to amplify the sequestration of U(VI) from aqueous environments.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yabin Zhang,Wenguang Zhang,Houxiang Yin,Yanlin Wang,Bingbing Wang,Lishuai Zong,Jinyan Wang,Xigao Jian
The robust human–machine interaction systems of the aerospace industry necessitate the development of thermal resistant wave-transparent composites, with a pivotal focus on organic resin matrix. However, enhancing the heat resistance of such materials while preserving other critical attributes has been a formidable challenge. In this study, a novel designed strategy of a dual-curing functional phosphorus-based phthalonitrile monomer (P-ALK-PN) has been proposed. The optimized curing temperatures for intra- or intermolecular Diels-Alder reactions of alkynyl groups and polyaddition reaction of cyano groups resulted in a homogeneous and highly crosslinked N-enriched phthalonitrile system. After curing at 450 °C, the resin, namely P-ALK-PN-450 °C, demonstrated exceptional thermal stability ( T 5% = 644 °C), thermo-oxidative stability ( T 5% = 554 °C), and char yield at 800 °C (90.7 % in N 2 and 67.5 % in air). Their quartz fiber reinforced composites (P-ALK-PN/QFs) were subsequently fabricated by the hot-pressing process. Upon post-curing at 420 °C, P-ALK-PN-420 °C/QF displayed elevated glass transition temperature (550 °C), flexural strength (319 MPa), and relatively low dielectric properties with a dielectric constant (D k ) of approximately 4.2 and a dissipation factor (D f ) less than 0.02 across a wide temperature ranging from 25 °C to 600 °C. Especially, it exhibited excellent flame retardancy (only a 6.7 % weight loss at ambient temperatures exceeding 1300 °C for 200 s) as well, stemming from release of eco-friendly inert gases (NH 3 ) and formation of a graphitized protective layer during pyrolysis. These promising results highlight the potential applications of P-ALK-PN resins in aerospace and high-performance engineering fields.
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