POLYHEDRON
·
2020
·
IF 2.343
Zhongmin Liu,Cong Wang,Yongchuan Wu,Longlong Geng,Xiuling Zhang,Dashuai Zhang,Hui Hu,Yongzheng Zhang,Xin Li,Wei Liu,Ping Na
The adsorption behavior of arsenic on adsorbent have been researched widely, but chemical adsorption of arsenic is uncommon. In this work, a kind of microporous metal-organic framework (MIL-125(Ti)) with columnar morphology and uniform size was solvothermally synthesized, and its chemical adsorption behavior and mechanism of arsenic were firstly investigated by experimental and simulation study. Remarkably, ultra-fast adsorption behavior and excellent arsenic removal capability was achieved. It takes only 20 min to rapidly remove 5 mg L −1 arsenic with 0.2 g L −1 MIL-125(Ti), which is far superior to the previously reported materials. Both experimental and simulation study results show that the adsorption of arsenic obeys a new chemical adsorption mechanism. Both As(III) and As(V) can easily replace the terephthalic acid ligand via competitive coordination and bind to the Ti active site of MIL-125(Ti). In addition, the reaction energy barriers for ligand substitution by H 2 O, As(III) and As(V) are 0.46, 0.33 and 0.15 eV, respectively, which further confirming that structure reforming of MIL-125(Ti) plays a key role for chemical adsorption. The study solves the difficulty of removing low concentration of arsenic and provides molecular-level understanding of the chemical adsorption mechanism of arsenic on MIL-125(Ti).
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2021
·
IF 5.316
Hongmei Chen,Yanyun Fan,Zheng Fan,Hongyan Xu,Danfeng Cui,Chenyang Xue,Wendong Zhang
Photocatalytic water splitting under irradiation by sunlight to achieve hydrogen with the participation of semiconductor materials is deemed as the most promising green and clean energy supply strategy. Hence, it is particularly important and emergency to design photocatalyst with both high activity and stability to perform high-efficiency hydrogen evolution reaction (HER). In this study, we report a competitive coordination strategy to modulate the electron and band structure of g-C 3 N 4 dramatically improving the HER kinetics. Experimental and density functional theory (DFT) calculations results inferred that the modified g-C 3 N 4 by copolymerizing urea and diaminodiphenyl sulfone can promote the effective separation of photogenerated electrons and holes, and simultaneously significantly increase the fluorescence lifetime of g-C 3 N 4 . Specifically, the hydrogen generation rate is 3.7 or 9.6 folds higher of the original carbon nitride at λ > 400 nm and λ > 420 nm, respectively. Additionally, the optimal catalyst exhibits a high apparent quantum yield (7.02%) when the incident wavelength is 420 nm as well as excellent stability. This work will shed a spick-and-span insight for conception and preparation of high-powered metal-free photocatalysts.
研究领域:
材料科学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Dingliang Dai,Jianhao Qiu,Guanglu Xia,Yong Tang,Zhonghao Wu,Jianfeng Yao
Core-shell Bi-MOF@BiOX (X = I, Br and Cl) hybrids were fabricated by a one-pot solvothermal strategy via regulating the concentration and type of halogen ions in the Bi-based CAU-17 synthesis. By virtue of the competitive coordination effect to Bi 3+ between CAU-17 and BiOX, CAU-17 was converted into another Bi-MOF with similar structures and compositions. Moreover, Bi 3+ plays the role of “bridge” and endows an intimate interface contact between BiOX and the Bi-MOF, which immensely expedites the charge and mass transportation. The obtained Bi-MOF@BiOX hierarchical heterostructures were applied to photocatalytic elimination of solo and mixed pollutants (Cr(VI)/tetracycline and Cr(VI)/o-nitrophenol), and exhibited favorable performances. Choosing Bi-MOF@BiOI as a typical example, the corresponding performances for Cr(VI) reduction, tetracycline and o-nitrophenol degradation in their solo systems are 14, 10, 8 times higher than those of CAU-17, and 13, 7, 5 times higher than those of BiOI under visible light, respectively. Of note, the above photocatalytic performances could be further improved in the coexisting environment of Cr(VI) and tetracycline or o-nitrophenol, which is attributed to the elevated charge separation efficiency caused by the timely consumption of photo-excited electrons and holes. This work gives some insights into the delicate design of MOF photocatalysts and their applications in environmental restoration.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
TALANTA
·
2023
·
IF 6.1
Yatian Cao,Xiaolong Gong,Le Li,Huihui Li,Xuanming Zhang,Dong-Yu Guo,Fuxiang Wang,Qinhe Pan
Bacillus anthracis spores can make humans infected with vicious anthrax, so it is significant to detect their biomarker 2,6-pyridinedicarboxylic acid (DPA). The development of dual-modal methods for DPA detection that are more flexible in practical applications remains a challenge. Herein, colorimetric xylenol orange (XO) was modified on fluorescent CdTe quantum dots (QDs) for dual-modal detection of DPA through competitive coordination. After the binding of XO on CdTe QDs via coordination with Cd 2+ , CdTe QDs displayed quenched red fluorescence and the bound XO was presented as red color. The competitive coordination of DPA with Cd 2+ made XO released from CdTe QDs, causing the enhanced red fluorescence of CdTe QDs and the yellow color of free XO. On this basis, DPA was rapidly (1 min) quantified through fluorescent and colorimetric modes within the ranges of 0.1–5 μM and 0.5–40 μM, respectively. The detection limits for DPA were calculated as low as 42 nM and 240 nM, respectively assigned to fluorescent and colorimetric modes. The level of urinary DPA was further measured. Satisfactory relative standard deviations (fluorescent mode: 0.1%–10.2%, colorimetric mode: 0.8%–1.8%) and spiked recoveries (fluorescent mode: 100.0%–115.0%, colorimetric mode: 86.0%–96.6%) were obtained.
研究领域:
生物化学
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分析化学
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医学诊断
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产品关联
DOI
PubMed
高影响因子
FOOD CHEMISTRY
·
2024
·
IF 8.5
Linglong Yi,Shangzai Wu,Guojian Ren,Qi Zhou,Ping Li,Yuan Wang,Xudong Tian,Danfeng He,Qinhe Pan
Glyphosate is a widely used herbicide in agriculture, leading to residues in food and water environments. These residues have been associated with heart disease and neurotoxicity. Therefore, it is urgent to develop new types of sensors for the detection of glyphosate residues. Here, a new coordination polymer, named as HNU-89 , is synthesized by the assembly of Eu 3+ and coumarin-3-carboxylic acid (HCCA). Benefiting from the hydrophobic ligands, HNU-89 can maintain its structure at pH 2–11. In view of that phosphoric groups in glyphosate molecules can coordinate with Eu 3+ and compete with the HCCA ligand, according to the competitive coordination, the interaction weakens the red fluorescence of HNU-89 simultaneously enhancing the blue fluorescence of HCCA, which achieves the ratio fluorescence response for glyphosate detection. The limit of detection (LOD) is 0.08 ppm, meeting the requirements as a sensor. Furthermore, HNU-89 was utilized to detect glyphosate in soybean, corn, rice and tap water.
研究领域:
分析化学
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF POWER SOURCES
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2025
·
IF 7.9
Xiao Jun Xu,Han Zeng,Mi Zhang,Bao Chen Han
Graphene oxide is covalently tethered to porphyrin derivative to prepare carbon based nano-material with photo-sensitive group modification as bio-molecule accommodation matrix. Graphene oxide with porphyrin derivative tailoring is proposed to fabricate Laccase-based electrode via a variety of mutual interactions including the competitive coordination. The microscopic, spectrometric, and electrochemical techniques are proposed to explore the impacts of the mutual interactions between incorporated Laccase and components of graphene oxide-photosensitive group assembly on the photo-electro-catalytic effect of such dual aggregation with enzyme entrapment . The novel intermediate species with distinguished spectroscopic and electrochemical idiosyncrasies could be engendered from the binding of Laccase with the porphyrin derivative. The coordination of enzyme with hetero-aromatic group would not decrease the affinity of immobilized protein to the dissolved substrate: di-oxygen molecules to great extent. The combination would bring on the aggrandizement in the band gap (1.5 eV) of nano-composite with Laccase attachment to depress the utilization efficiency of the external irradiation. The generated intermediate shows the inferior dynamics of charge transportation and unfavorable electrochemical activity. Such competitive ligation of Laccase with hetero-atoms in the porphyrin ring would augment the active energy of the subsequent transformation. In general, the competitive ligation of integrated Laccase molecules with hetero-atoms in porphyrin derivative would not only decrease the charge efficiency for cofactor within redox enzyme (0.065 s −1 ) but also depress the binding-transformation kinetics of active sites in Laccase (i.e. oxygen-binding sites, tri-nuclear copper cluster) .
研究领域:
材料科学
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生物化学
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纳米技术
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电化学
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催化
✓ 已验证
产品关联
DOI
高影响因子
FOOD CHEMISTRY
·
2025
·
IF 9.8
Ying Huang,Xiangrong Liu,Tiantian Shen,Wang Li,Jiali Ren,Haiyan Zhong
The detection techniques for glyphosate residues have garnered attention due to the potential toxicity associated. Herein, we introduced a fluorescent “turn-on” strategy, leveraging competitive coordination with iron, for glyphosate detection. We synthesized iron-based metal-organic frameworks (Fe-MOFs) at room temperature. Among them, 2,5-dihydroxyterephthalic acid (DOBDC) acted as a ligand to produce strong fluorescence, and iron ions acted as a quencher to quench the fluorescence of DOBDC. Another ligand, 2-nitroterephthalic acid, contained nitro quenching of the fluorescence, giving it a lower background. Glyphosate competed with the ligands for ions, weakening the interaction between ions and the ligands. This disruption restored the fluorescence emission at 535 nm, enabling glyphosate detection. To facilitate field application, Fe-MOFs were encapsulated within agarose to create a functional hydrogel. Glyphosate penetrated the hydrogel and resulting in fluorescence “turn-on”. Remarkably, this method facilitated visual detection through smartphone photography coupled with RGB (red/green/blue) analysis, offering a user-friendly and portable solution.
研究领域:
环境科学
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分析化学
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材料科学
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传感器和检测技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MICROCHIMICA ACTA
·
2023
·Vol. 191
·期 1
·1-9
·
IF 5.7
Huang Xuemin,Chen Haiyan,Huang Rui,Shi Yuande,Ye Ruihong,Qiu Bin
Benefit from the strong coordination property, lanthanide metal ions have been used as competitive reagents to modulate the fluorescence changes of the system. However, lanthanide metal ions as inducers for aggregation-induced emission enhancement in nanosystems is rare. Herein, we report a “turn on–off-on” fluorescent switch for cascade detection of acid phosphatase (ACP) and adenosine triphosphate (ATP) based on the competitive coordination of samarium ions (Sm 3+ ). Novel copper nanoclusters (CuNCs) with long wavelength emission (614 nm) stabilized by glutathione (GSH) and glycylglycine (Gly-Gly) have been confirmed to have AIE property. With the continuous aggregation of GSH/Gly-Gly CuNCs under the induction of Sm 3+ , the fluorescence of the system increased to achieve the “turn-on” process. The coordinated behaviour between Sm 3+ and GSH/Gly-Gly CuNCs is discussed. Due to the strong metal coordination ability of ATP, the Sm 3+ coordinated with the GSH/Gly-Gly CuNCs is competed out, resulting in the fluorescence “turn-off” process of the system. As the substrate of enzymatic hydrolysis of ACP, with the continuous hydrolysis of ATP by ACP, Sm 3+ coordinates with GSH/Gly-Gly CuNCs again, which leads to the AIE effect and realize the fluorescence "turn-on" process of the system. This strategy results in ATP linear range of 0.508 ~ 120.0 μM with a detection limit of 0.508 μM (S/N = 3) and ACP linear range of 0.011 ~ 30.0 U·L −1 with a detection limit of 0.011 U·L −1 (S/N = 3). Application to biologic samples was successful. Graphical Abstract
研究领域:
分析化学
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生物化学
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纳米技术
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生物检测
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry B
·
2024
·
IF 6.1
Ke Wang,Sicheng Zhai,Yuanyuan Qin,Mengke Hao,Siqi Su,Shuming Li,Xuexue Tang
Controlled drug release with on demand holds great promise for cancer therapy. Light-degradable nanocarriers have gained increasing attention for designing controllable drug delivery systems due to their spatiotemporally controllable properties. Herein, a high luminescent and light-degradable nanocarrier is constructed by intercalating glutathione-capped gold nanoclusters (AuNCs) into zeolitic imidazolate framework-8 (ZIF-8) via competitive coordination assembly, named as AuNC@ZIF-8, for light-triggered drug release. Glutathione-capped AuNCs and 2-methylimidazole (MIm) competitively coordinated with Zn2+ to form AuNC@ZIF-8 via one step process in aqueous solution. Specifically, the obtained AuNC@ZIF-8 has a high quantum yield of 52.96 % and displays a distinctive property of photolysis. The competitive coordination interactions within AuNC@ZIF-8 were evidenced by X-ray diffraction and X-ray photoelectron spectroscopy, in which Zn2+ strongly coordinated with the N of MIm and weakly coordinated with the carboxyl/amino groups in glutathione of AuNCs. Under light irradiation, the Au-S bond on AuNCs breaks, enhancing the coordination ability between carboxyl/amino groups and Zn2+ enhance. This leads to the collapse of the crystal structure of AuNC@ZIF-8 and subsequent fluorescence quenching. Additionally, AuNC@ZIF-8 is successfully employed as luminescent nanocarriers of anticancer drugs to form drug-AuNC@ZIF-8, in which three typical anticancer drugs are selected due to different coordination interaction. The obtained smart drug-AuNC@ZIF-8 can be effectively internalized into HeLa cells and degraded in response to blue light, with negligible dark cytotoxicity and high light cytotoxicity. This study highlights the crucial role of competitive coordination interactions in synthesizing functional materials with fluorescence efficiency and photolytic properties.
研究领域:
纳米技术
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材料科学
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癌症研究
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药学
·
光化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）