Frontiers in Chemistry
·
2022
·
IF 5.545
Liu Yangqing,Sun Jingwen,Fan Lan,Xu Qi
Subnanometer noble metal clusters have attracted much attention because of abundant low-coordinated metal atoms that perform excellent catalytic activity in various catalytic processes. However, the surface free energy of metals increases significantly with decreasing size of the metal clusters, which accelerates the aggregation of small clusters. In this work, new Schiff base–imidazole-functionalized MOFs were successfully synthesized via the postsynthetic modification method. Highly dispersed Pd clusters with an average size of 1.5 nm were constructed on this functional MOFs and behaved excellent catalytic activity in the Suzuki coupling of phenyboronic acid and bromobenzene (yield of biaryl >99%) under mild reaction conditions. Moreover, the catalyst can be reused six times without loss of activity. Such catalytic behavior is found to closely related to the surface functional groups that promote the formation of small Pd0 clusters in the metallic state.
研究领域:
材料科学
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催化化学
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DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Chenghan Ji,Mujian Xu,Hang Yu,Lu Lv,Weiming Zhang
The development of heavy metal adsorbents with high selectivity has become a research hotspot due to the interference of coexisting ions (e.g., Na + , Ca 2+ ) in the actual wastewater, but the more difficult regeneration caused by high adsorption selectivity severely limits its practical applications. Herein, a carboxyl adsorbent, MIL-121, demonstrated high adsorption selectivity for heavy metals at 10,000 mg/L of Na + (removal > 99% for Cu 2+ ) as well as unexpected easy regeneration (desorption > 99%) at low H + concentration (10 −3.5 –10 −3.0 M), which is hundreds of times lower than that of ever reported selective adsorbents (> 10 −1 M H + ). X-ray photoelectron spectrometry (XPS), extended X-ray absorption fine structure (EXAFS) coupled with Density functional theory (DFT) simulation unveil that the -COOH groups in MIL-121 for heavy metals adsorption is specific inner-sphere coordination with higher binding energy (1.31 eV for Cu), and less energy required for regeneration (0.26 eV for H). Similar high selectivity and easy regeneration were also satisfied with other heavy metals (e.g., Pb 2+ , Ni 2+ ), and removal of heavy metals remained > 99% in 10 consecutive adsorption-desorption cycles. For actual copper electroplating wastewater treatment , MIL-121 could produce ~ 3600 mL clean water/g sample, outperforming 300 mL that of the benchmark commercial adsorbent D-113. This study shows the potential of MIL-121 for heavy metal wastewater treatment and provides mechanistic insight for developing adsorbents with high selective adsorption and easy regeneration.
研究领域:
环境科学
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材料科学
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DOI
PubMed
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2023
·Vol. 332
·期 10
·4167-4177
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IF 1.6
Peng Yinyin,Pan Ting,Chen Chuang,Zhou Mi,Liu Derong,Feng Jian,Xiong Wei,Liu Ning,Yuan Guoyuan
In this work, MOFs materials functionalized (HC-MOFs) with heterocyclic ligands (thiophene-TPC, pyrrole-PCA and furfural-FUR) were prepared by a one-step method and used for cobalt ion separation studies. The results showed that the maximum adsorption of cobalt ions by the three adsorbents was 141.0 mg/g (UiO-66-TPC), 146.0 mg/g (UiO-66-PCA), and 150.6 mg/g (UiO-66-FUR), respectively, at pH 8.3 and a temperature of 298 K. In addition, The HC-MOFs showed good stability under different doses (0 ~ 200 kGy) of γ-ray irradiation and have great potential for application in the separation of practical radioactive wastewater containing 60 Co.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
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IF 7.3
Hongqi Liang,Fenglong Chen,Zhizhuo Liu,Litao Tian,Jingmei Xu
The design and preparation of low-cost and high-stability proton exchange membranes (PEMs) play an indispensable role in sustainable development and application expansion. In this study, sulfonic acid-amino difunctionalized hydrophilic metal–organic frameworks (MOFs) (named as TA-SNU6) were designed and synthesized as proton transport carriers to be incorporated into sulfonated poly(aryl ether ketone sulfone) (SPAEKS) to obtain high proton conductivity and single-cell performance. The experimental results show that abundant hydroxyl and acid–base groups significantly increase the proton transport efficiency in PEMs and improve the hydrophilicity and electrochemical performance of PEMs. The single-cell performance of the STSN-1% membrane was about 1.8 W cm–2. The proton conductivity was up to 190 mS cm–1, the mechanical properties were significantly improved, and the tensile strength reached 48 MPa. SPAEKS polymer with a specified degree of sulfonation was prepared by a stepwise polycondensation reaction, which showed excellent comprehensive properties after adding TA-SNU6 fillers. The STSN-1% composite membrane performs better than Nafion 211 and Nafion 117 in fuel cells. Therefore, it can be seen that this work has achieved certain results, which makes PEMs have excellent electrochemical performance, and provides a reference for the development of high-performance PEMs.
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Ying Zhou,Donghui Wang,Dingnan Wang,Yang Wang,Yang Li,Jie Li,Yiming Zhang
Mimetic recognition materials for rapid and selective analysis of foodborne contamination from complex foodstuff becomes a hot research topic in the field of food safety. In this work, borate-affinity-functionalized MOF/molecularly imprinted polymer paper-based microfluidic chips (FSU-BA@MIP) were prepared by growing functionalized MOFs on paper surface with 3-carboxyphenylboronic acid (3-CPBA) as the ligands, followed by coating of a MIP layer of salbutamol (SAL) through a borate-affinity surface imprinting strategy. Using the obtained paper-based chip as a mimetic recognition and specific enrichment module, the fluorescence sensing platform achieved visual rapid quantitative analysis of SAL with a linear range of 0.1 × 10 −2 –5.0 mg L −1 . The limits of detection and quantification were calculated to be 0.095 and 0.290 μg kg −1 , respectively, and the sample loading via lateral flow aid could be completed within 30 min. The obtained MOFs/MIPs paper chips provide an effective way for the rapid analysis of harmful contaminants from different animal-derived foods.
研究领域:
食品安全
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分析化学
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产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2025
·Vol. 49
·期 23
·9663-9668
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IF 2.5
Wenhui Yao,Yongkui Chen,Xiaowei Guo
With the wide application of gold as a high-value resource, the recycling of gold has received considerable attention. Owing to the functional active sites, tunable pore size and designable structures, metal–organic frameworks (MOFs) have aroused significant curiosity in gold-recycling. However, designing MOFs with both remarkable adsorption capacity and selectivity for Au(III) is highly desirable but challenging. In this work, two hydroxy-modified UiO-66-type MOFs: UiO-66-(OH)2 and UiO-66-OH have been prepared for rapid and selective adsorption of gold ions from aqueous solution. Significantly, UiO-66-(OH)2 was found to exhibit a remarkable gold adsorption capacity of 1570 mg g−1 (pH = 6) compared with UiO-66-OH (520 mg g−1) under uniform conditions. Furthermore, UiO-66-(OH)2 still exhibited excellent gold adsorption efficiency in the presence of other interfering ions. Mechanism analyses revealed that Au(III) was partly transformed to Au(0) by the reducing action of –OH on the framework in the gold adsorption process. Importantly, the MOF materials can be well regenerated by soaking in hydrochloric acid–thiourea aqueous solution.
研究领域:
材料科学
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环境化学
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无机化学
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可持续资源回收
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
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IF 7.7
Fan Yang,Hui-Hui Xie,Fan Du,Xiaomin Hou,Si-Fu Tang
Enzyme immobilization is an effective strategy for achieving efficient and sustainable enzyme catalysis. As a kind of promising enzyme-loading materials, the systematic research on zirconium based metal organic frameworks (Zr-MOFs) about immobilization performance at molecular level is still in its initial stage. In this work, UiO-66 was functionalized with various groups (-H, -NH 2 , -COOH, -OH, -2OH) for the immobilization of cytochrome c (Cyt c) and antioxidant enzyme catalase (CAT). Then the effects of surface-functionalized UiO-66 derivatives on the loading efficiency, enzyme stability and catalysis kinetics were systematically investigated. In addition, the affinity constants of Cyt c and CAT towards UiO-66-series MOFs carriers were also compared. The results have shown that hydroxyl group functionalized UiO-66 represents the highest enzyme loading capacity, enhanced activity and improved stability for Cyt c and CAT possibly due to high surface area and suitable microenvironments as well as enhanced affinity towards the enzymes provided by the introduction of a single hydroxyl group. Our research would foresee immense potential of MOFs in engineering biocatalysts.
研究领域:
材料科学
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生物催化
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化学工程
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生物化学
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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
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IF 8.6
Zhi Hu,Shucheng Liu,Nana Tang,Xuan Zhang,Jianming Pan
The main obstacles of recognition of flavoniods are low concentration and complexity of extract wastewater solutions. The structural and stability limitation of the sorbents is the significant reason for the difficulty in increasing the adsorption amount in the separation system. Hereon, a novel hierarchical-pore boronic acid-functionalized-MOFs based on macroporous organo/hydro copolymers (CPs@H-UiO-66-NH 2 @BA) were firstly fabricated through the triple sacrificial cross-linking strategy, which allowed the formation of multiple hydrogen bond networks (i.e. main crosslinked networks and weak crosslinked networks) at oil–water interface. Noticeably, the MOFs with polymer chain entanglement effects as a physical sacrificial cross-linking network, significantly enhancing the mechanical properties. The maximum equilibrium binding capacity of CPs@H-UiO-66-NH 2 @BA was 40.93 µmol g −1 for NRG at 308 K. Furthermore, it also showed superior regeneration capacity capability (only 7.81% loss) after six cycles. Meanwhile, they had a stronger selectivity towards NRG. It can effectively purify the low purity of the actual sample ground to 92.68%. It is anticipated that in-situ the introduction of nanoboronic-functionalized MOFs construction into copolymers would hold great promise in the selective capture of target flavonoids in actual samples.
研究领域:
材料科学
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化学工程
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分析化学
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产品关联
DOI
高影响因子
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