Nature Communications
·
2025
·Vol. 16
·期 1
·1-16
·
IF 15.7
Liu Ya,Yang Jiajia,Wang Yuxian,Zhu Wanli,Hu Kunsheng,Liu Zhang,Yeung Kinglun,Zhu Zhong-Shuai,Chen Chunmao,Duan Xiaoguang,Wang Shaobin
Compositional heterogeneity in metal/nitrogen-doped carbons (M-N-Cs) complicates the fundamental elucidation of the intricate interplay between the active metal species that rule the reactivity of single atomic catalysts (SACs). This study unveils the electronic disruptions of cobalt nanoparticles (Co NPs) to the catalytic behaviors of cobalt single-atom (Co SA). The intense electronic communications between high-density Co NPs and Co SA sites lead to dissociation O 3 on the high-spin Co SA sites to generate surface-confined hydroxyl radicals ( • OH). However, the tandem electron transfer yields superoxide radical (O 2 •– ) with low reactivity and remarkably reduce ozone utilization efficiency (OUE). In contrast, independent Co SA sites far or free from adjacent Co NPs induce a nonradical O 3 activation regime, which markedly improves electron utilization efficiency (~2.9-fold), OUE ( ~ 3.0-fold), and turnover frequency (TOF, ~2.5-fold) of Co SA. The nonradical catalytic ozonation process demonstrates high adaptability to complex water matrices and maintains long-term stability in the treatment of real petrochemical wastewater. The deciphered electronic interplays between metal nanoparticles and single atom sites advance a new paradigm to regulate the selectivity of single atom catalysis.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2026
·
IF 5.4
Zina Zhang,Kaiyue Fan,Tengda Shi,Tong Hao,Jiaqi Li,Yanan Yang,Yu Bian,Hong Zheng
The key to removing and detecting trace Hg (II) in water is to achieve rapid adsorption and high adsorption capacity of the adsorbent while maintaining the simplicity and safety of the adsorbent preparation process. Herein, we report a post-modification of covalent organic frameworks by medical antidote dimercaprol (DMC-COF) for efficacious removing and detection on trace Hg (II) in water. The as-prepared DMC-COF showed excellent selectivity to trace Hg (II) and fast adsorption dynamics, which was attributed to the abundance of sulfhydryl and hydroxyl sorption sites in the COF mesopores and on the COF surface. The effluent concentration of Hg(II) coexisting with Ca(II) reduced from 30 μg·L −1 to the permissible limit (1 μg·L −1 ) of potable water standard within 30 s. The sorption equilibrium was achieved during 3 min and the adsorption rate reached over 98 %. The material also showed a wide applicable pH range (3.5–9.5), excellent regeneration feasibility and selectivity of Hg(II) coexisting with a wide range of heavy metals in tap water, and the effluent concentration of Hg(II) coexisting with trace of As(V), Cr(VI), Cd(II) and Pb(II) could reduce from 30 to 0.19 μg·L −1 during 10 min. Moreover, Hg(II) of 3, 6, 10 and 30 μg·L −1 in tap water could be achieved to meet the WHO standard within 1 min. Meanwhile, its conjugated framework could be used as a signal sensor for rapid testing for low concentration Hg(II) in water, with a fluorescence detection limit of 1.06 mg·L −1 . DFT calculations yielded the optimized structure of DMC grafted onto COF-V, revealing that Hg²⁺ and Hg(OH)₂ primarily adsorbed at the -S and -SH sites, predominantly through van der Waals interaction, whereas Hg(OH)⁺ mainly adsorbed at all the -S, -SH and -OH sites, governed by notable attraction.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2020
·
IF 3.306
Haochi Liu,Jie Ding,Ligang Chen,Lan Ding
A novel approach was proposed to prepare carbon dots (CDs) by acid carbonization and hydrothermal treatment of pork rib bones from food waste. The synthesized animal waste biomass CDs have the merits of eco-friendly, superior fluorescence properties and biocompatibility. The fluorescence of animal waste biomass CDs could be quenched efficiently by dithizone due to the coordination effect. With the addition of dimethoate, the dithizone ligands at CDs are replaced by hydrolysates, and hence the fluorescence is recovered. Thus, a sensing platform was constructed based on the coordination-originated fluorescence of animal waste biomass CDs which can sensitively and selectively detect dimethoate due to a simple displacement mechanism. Upon optimal conditions, the detection limit of dimethoate is 0.064 μM. The linear ranges were obtained in a range of 0.15 μM–5.0 μM. The method is rapid, convenient and environmentally acceptable that can directly detect dimethoate in water samples with recoveries of 93 %–105 %, and the relative standard deviations (RSDs) were 2 %–6 %, respectively. This simple strategy can be used to develop the fluorescence recovery sensors for chemical detection.
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Journal of Food Measurement and Characterization
·
2023
·
IF 3.4
Du Huan,Li Tao,Xue Qiaoli,Tian Yang,Hu Yongjin
Moringa oleifera leaves are potentially benign sources of natural folates, thus a reliable folate extraction protocol is necessary, which directly affects the accuracy of subsequent determination of total folates or various folate derivatives. With this aim, process variables including antioxidants, extraction buffer pH, Moringa oleifera leaves powder (MOLP)/extraction buffer ratio, heating extraction time, amounts of α- amylase, protease and rat serum, and also incubation time of rat serum were investigated and optimized by response surface methodology (RSM). It is interesting that no positive influence of α- amylase or protease solution was observed in this study, consequently a single-enzyme treatment was used. An average folate level of 1190.06 µg/100 g dry matter was achieved by microbial assay under the optimized conditions of extraction buffer pH 7.0, MOLP/extraction buffer ratio 1:24 (g/mL), rat serum 350 µL, digest time 2.0 h, in good agreement with the value predicted by quadratic model. In addition, the validity of protocol established in this study was confirmed. The intra-day precision (relative standard deviation) varied between 1.42% with 1.84%, inter-day precision varied in the range of 1.34–2.25%. The average recoveries were in the range of 101.56–103.27%. Besides, the matrix effects ranged from 101.41 to 103.34%. The protocol could provide a reference to fairly evaluate folates in Moringa oleifera leaves from diverse sources, and even in other leafy plants. Meanwhile, Moringa oleifera leaves with high folate level seem to have tremendous potential to increase nutritional value of foods as well as to enhance regional economies.
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JOURNAL OF HAZARDOUS MATERIALS
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2019
·
IF 7.65
Wei Jiang,Qiang Xu,Xionghui Wei
It is first reported herein that cobalt(II) complexes solution of monothiol-containing multidentate ligands are used to remove low concentration of nitric oxide (NO). These chelating ligands are water-soluble amines, alcohols or acids which containing at least one -SH group, include those of cysteine, mercaptosuccinic acid, mercaptoethanesulfonate, mercaptopropionic acid and the like. These -SH compounds when coordinated with cobalt ions, forming complexes are very effective for NO removal. The results indicate that the side group (methyl, carboxyl, carboxymethyl) on α-carbon atom of ligands contribute to the denitration of the chelate solution, whereas the substituents on sulfur atom of ligands deactivate the complexation system. In addition, we have found that several monothiol compounds with simple molecule structure and low cost exhibit good performance in denitration, and some of cobalt thiol complexes are more valuable in removing NO than ferrous thiol complexes.
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APPLIED SURFACE SCIENCE
·
2015
·
IF 2.711
Lytuong Tran,Pingxiao Wu,Yajie Zhu,Shuai Liu,Nengwu Zhu
A novel approach to prepare adsorbents for Hg(II) uptake from aqueous media based on the grafting of dimercaprol (BAL), containing thiol and hydroxyl groups, onto the natural montmorillonite and vermiculite was investigated concerning the evaluation of the adsorption capacity. The kinetic study showed that the adsorption process abided by pseudo-second-order model. The adsorption behavior of Hg(II) onto the obtained samples fitted well with Langmuir isotherm model, exhibiting an enhanced maximum adsorption capacity of 8.57 and 3.21 mg g −1 for BAL-Vm and BAL-Mt, respectively. The feasibility of Hg(II) uptake onto the the samples was studied thermodynamically and the calculated coefficients such as Δ H , Δ S and Δ G indicated a physical and spontaneous process. The pH values and coexisting cations had a great influence on Hg(II) removal, confirming the optimal pH value of 4.0–5.0 and the negative correlation between the ionic strength and the adsorption capacity of Hg(II). In general, BAL-Vm possessed a higher efficiency of Hg(II) uptake than BAL-Mt, contrary to that of the pristine clays. The pristine and functionalized materials were investigated by XRD, FTIR, BET, SEM and zeta potential analysis to gain in-depth insight into the structure and surface morphology. The results showed that BAL was successful grafted on montmorillonite and vermiculite surface, providing plentiful adsorption sites as chelating ligands. The mechanisms of Hg(II) adsorption on these samples could be further explained as ion exchange and electrostatic attraction for Vm and Mt, and formation of complexes for BAL-Vm and BAL-Mt.
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INORGANICA CHIMICA ACTA
·
2017
·
IF 2.002
Xiujuan Jiang,Hailong Wang,Yonggang Feng,Erxing Gu,Xiaoming Liu
Three diiron carbonyl complexes with different carbonyl ligands have been synthesized. Pentacarbonyl and tetracarbonyl complexes 2 and 3 were prepared by the substitution of the bound CO of complex 1 by PPh 3 . The photo-induced CO-releasing behaviours of these complexes correlate linearly to their reduction potentials and further to the energy level of their LUMOs. The more negative the reduction potentials, the more reactive the complexes. The photo-induced CO-release can be further promoted when a nucleophile is presented such as thiopronin.
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PLoS One
·
2015
·Vol. 10
·期 8
·e0136450
·
IF 3.234
Guyue Cheng,Bei Li,Chenxi Wang,Hongfei Zhang,Guixia Liang,Zhifei Weng,Haihong Hao,Xu Wang,Zhenli Liu,Menghong Dai,Yulian Wang,Zonghui Yuan
Quinoxaline 1,4-di- N -oxides (QdNOs) are widely known as potent antibacterial agents, but their antibacterial mechanisms are incompletely understood. In this study, the transcriptomic and proteomic profiles of Esch erichia coli exposed to QdNOs were integratively investigated, and the results demonstrated that QdNOs mainly induced an SOS response and oxidative stress. Moreover, genes and proteins involved in the bacterial metabolism, cellular structure maintenance, resistance and virulence were also found to be changed, conferring bacterial survival strategies. Biochemical assays showed that reactive oxygen species were induced in the QdNO-treated bacteria and that free radical scavengers attenuated the antibacterial action of QdNOs and DNA damage, suggesting an oxidative-DNA-damage action of QdNOs. The QdNO radical intermediates, likely carbon-centered and aryl-type radicals, as identified by electron paramagnetic resonance, were the major radicals induced by QdNOs, and xanthine oxidase was one of the QdNO-activating enzymes. This study provides new insights into the action of QdNOs in a systematic manner and increases the current knowledge of bacterial physiology under antibiotic stresses, which may be of great value in the development of new antibiotic-potentiating strategies.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2015
·
IF 3.313
Diyang Zhu,Zhiyin Xiao,Xiaoming Liu
A number of fibrous membranes with cellulose acetate as a matrix and functionalised with diiron mimics of the diiron subunit of [FeFe]-hydrogenase were prepared by electrospinning technique . Four mimics, [Fe 2 (μ-edt) (CO) 6 ] ( 1 ), [Fe 2 {μ-SCH 2 CH(CH 2 OH)S}(CO) 6 ] ( 2 ), [Fe 2 {(μ-S) 2 (C 6 O 2 H 4 )}(CO) 6 ] ( 3 ) and [Fe 2 {μ-SCH 2 CH(OH)CH 2 (OH)} 2 (CO) 6 ] ( 4 ), bearing 0, 1, 2 and 4 hydroxyl group(s) were incorporated into the electrospun fibrous membranes ( EFM s). To improve the conductivity of the EFM s, graphene oxide was chemically gratified onto cellulose acetate. The resultant EFM s membranes were characterized using infrared spectroscopic, thermogravimetric and scanning electron microscopic techniques. The electrochemical behaviours and electrocatalytic performance on proton reduction of the membrane electrodes assembled from the EFM s showed in aqueous media that the membrane ( M2 ) containing complex 2 is most durable and exhibited the best catalytic performance. To the electrospinning system containing complex 2 was further doped with basic polymer PEI to enhance tentatively proton transfer during the electrocatalysis of proton reduction. Our results showed that the presence of PEI in the EFM s did improve the electrocatalytic performance of proton reduction, presumably due to the enhancement in proton transfer in the catalysis.
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DALTON TRANSACTIONS
·
2014
·Vol. 43
·期 26
·9968-9975
·
IF 4.097
Xiujuan Jiang,Li Long,Hailong Wang,Limei Chen,Xiaoming Liu
The CO-releasing behaviours of nine diiron carbonyl complexes (1–9) were examined via the substitution reaction of cysteamine (CysA), of which complex 4 was reported recently. These complexes fall into three categories, the diiron core bridged by two thiolates, a dithiolate and 1,8-naphthalene dithiolate. Our results reveal that the CO-releasing rates of these complexes are highly dependent on their structures. Complexes (2–4) bearing two monothiolates as their bridging linkage (“open” form) are more vulnerable to decomposition upon nucleophilic substitution reactions compared with complexes (6–9) that possess a dithiolate as their bridging linkage. When the bridging linkage lacks an electron-donating group (complex 1), the metal centre is less negatively charged as revealed by DFT calculation, and thus it exhibits fast substitution reaction with CysA to release CO. A linkage with conjugating nature (5) shows a similar effect because electron density on the metal centre decreases due to electron-density diverting from the metal centre into the naphthalene moiety. Kinetic analysis suggests that CO-releasing at the first stage of these complexes is a first-order reaction.
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MOLECULAR PHARMACEUTICS
·
2025
·
IF 4.5
Hui Xiong,Jingxue Yan,Jun Zhang,Yuhang Jiang,Xiaoqin Chi,Hongyu Lin,Jinhao Gao
The severe occurrence and mortality of cancer and the gradually increasing failure rate of traditional chemotherapeutic agents call for the search for alternative strategies for cancer therapy. Herein, we report the development of a small-molecule prodrug TAO-CA by conjugating a trivalent organoarsenical (TAO) with a natural product cinnamaldehyde (CA) via an acetal linkage. This prodrug is able to be activated under the mildly acidic environment of the tumor to release the two parent drugs for simultaneously inhibiting the activity of thioredoxin reductase (TrxR) and reducing the cellular level of glutathione (GSH), resulting in intracellular redox dyshomeostasis and consequent cancer cell apoptosis for effective inhibition of tumor growth. The mechanism and efficacy of this prodrug have been validated by a series of in vitro and in vivo experiments, demonstrating the promising potential of our strategy, the integration of the prodrug approach, and synergistic redox dyshomeostasis induction for effective cancer therapy.
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