ANALYTICA CHIMICA ACTA
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2024
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IF 5.7
Xiangyu Ma,Yaoying Cui,Kexing Zhu,Xiufang Zhu,Lijing Zhang,Liming Guo,Liangdong Feng,Jiadong Zhang,Yihong Wang,Ling Xia
Background Nanozymes , a new class of nanomaterials , have emerged as promising substitutes for enzymes in biosensor design due to their exceptional stability, affordability, and ready availability. While nanozymes address many limitations of natural enzymes, they still face challenges, particularly in achieving the catalytic activity levels of their natural counterparts. This indicates the need for enhancing the sensitivity of biosensors based on nanozymes. The catalytic activity of nanozyme can be significantly improved by regulating its size, morphology, and surface composition of nanomaterial. Results In this work, a kind of hollow core-shell structure was designed to enhance the catalytic activity of nanozymes. The hollow core-shell structure material consists of a nanozymes core layer, a hollow layer, and a MOF shell layer. Taking the classic peroxidase like Fe 3 O 4 as an example, the development of a novel nanozyme@MOF, specifically p-Fe 3 O 4 @PDA@ZIF-67, is detailed, showcasing its application in enhancing the sensitivity of sensors based on Fe 3 O 4 nanozymes. This innovative nanocomposite, featuring that MOF layer was designed to adsorb the signal molecules of the sensor to improve the utilization rate of reactive oxygen species generated by the nanozymes catalyzed reactions and the hollow layer was designed to prevent the active sites of nanozymes from being cover by the MOF layer. The manuscript emphasizes the nanocomposite's remarkable sensitivity in detecting hydrogen peroxide (H 2 O 2 ), coupled with high specificity and reproducibility, even in complex environments like milk samples. Significance and novelty This work firstly proposed and proved that Fe 3 O 4 nanozyme@MOF with hollow layer structure was designed to improve the catalytic activity of the Fe 3 O 4 nanozyme and the sensitivity of the sensors based on Fe 3 O 4 nanozyme. This research marks a significant advancement in nanozyme technology, demonstrating the potential of structural innovation in creating high-performance, sensitive, and stable biosensors for various applications.
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PubMed
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
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2025
·Vol. 39
·期 3
·e70008
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IF 0
Yawen Wu,Xueying Hou,Ao Li,Ruijian Li,Qingqing Yang,Shaohua Jiang,Jing yu Hu,Qingliang You,Rui Guo
As the amount of tetrachlorobisphenol A (TCBPA) that causes potential adverse effects on human health in the environment is continually increasing. It is therefore important to develop new materials for the adsorption or degradation of these compounds using various techniques. In this study, two novel magnetic recyclable composite catalysts Zr–NiFe 2 O 4 @ZIF-67 and Zr–NiFe 2 O 4 @ZIF-8 were synthesized. These catalysts degraded tetrachlorobisphenol A (TCBPA) in water by activating peroxydisulfate (PDS)/peroxymonosulfate (PMS), respectively. The results show that the Zr–NiFe 2 O 4 @ZIF-67-5%/LED/(NH 4 ) 2 S 2 O 8 system can degrade 95% of TCBPA (20 mg/L) within 30 min, whereas the Zr–NiFe 2 O 4 @ZIF-8-10%/LED/KHSO 5 system degrades 90% of TCBPA within 30 min. In instances of metal leaching at low concentrations, nickel and iron ions declined to 0.008 mg·L −1 , TCBPA exhibits highly efficient and sustainable catalytic properties, maintaining over 80% efficacy across six cycles. The online infrared test experiment results showed the major functional groups disappearing within approximately 130 s. The results of electron paramagnetic resonance and free-radical-quenching experiments showed that SO 4 ˙ − , ˙OH, 1 O 2 , and O 2 ˙ − were involved in the degradation of TCBPA. The possible degradation paths are isomerization polymerization, dechlorination, hydroxylation, ring-opening by oxidation, and further transformation into small molecules of acids, aldehydes, alcohols and other compounds. Thus, in this study, a reliable technique for the degradation of halogenated bisphenol compounds is developed. Overall, the photocatalytic degradation of organic pollutants in water utilizing polymetallic composites as catalysts represents an innovative approach to water treatment, demonstrating enhanced catalytic activity and recyclability, with promising prospects for significant advancements in both theoretical research and practical applications.
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Molecular Catalysis
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2024
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IF 3.9
Na Wei,Lin Liu,Jia-Qi Chu,Ting Fang,Zheng-Bo Han,Zhen Zhao
Metal-organic frameworks (MOFs) are widely studied for cycloaddition of CO 2 as a heterogeneous catalyst, because of their potential Lewis acidic sites and adjustable porous structure. However, most of them exhibit good catalytic performance need the assistance of nucleophilic co-catalysts. Herein, a novel MOFs and porous organic polymers (POPs) hybrid catalyst, core-shell ZIF-67@PDB-Br, is constructed by a convenient synthetic strategy, which possesses abundant Lewis acidic sites, imidazole cations and nucleophilic centers and shows robust chemical and thermal stability. This material demonstrates high-efficient catalytic activities and recyclability in the cycloaddition of CO 2 and propylene oxide without co-catalysts, the conversion and selectivity can reach 94.1 % and 99.0 %, respectively (100 °C, 1.0 MPa CO 2 pressure). Furthermore, the effects of the temperature, pressure, amount of catalyst and thickness of POPs shell on the catalytic activity were investigated. This study provides a viable direction for the development of synergistic heterogeneous catalysts for fixation of CO 2 without co-catalysts.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Ziyi Li,Jia Xiong,Hang Song,Shuchang Liu,Yufei Huang,Yangqiang Huang,Geoffrey I. N. Waterhouse,Ziyun Wang,Yu Mao,Zhiwu Liang,Xiao Luo
To enhance the photocatalytic efficiency of ZIF-67 (Zeolitic Imidazolate Framework-67), we integrated it with Ti 3 C 2 T x MXene through in-situ synthesis and assessed the effects of different MXene concentrations on photocatalytic activity. We identified ZIF-67/Ti 3 C 2 T x MXene as the optimal catalyst (denoted as ZT-450), yielding CO, CH 4 , and H 2 at 62.7, 6.7, and 7.3 μmol g −1 , respectively. The CO productive rate achieved by ZT-450 exhibits a substantial enhancement, outperforming both ZIF-67 and Ti 3 C 2 T x by factors of 16.1 and 4.8, respectively. After introducing Ti 3 C 2 T x in ZIF-67, CO 2 adsorption ability achieves 127.90 μmol g −1 , much higher than those of pure ZIF-67 and Ti 3 C 2 T x . Combining Density Functional Theory (DFT) calculations, we established that introducing Ti 3 C 2 T x in ZIF-67 facilitates rapid electron transfer and improves light absorption, CO 2 activation. In-situ DRIFTS measurements of photocatalytic CO 2 reduction reaction (CO 2 RR) on ZIF-67/Ti 3 C 2 T x MXene composite were employed to reveal the emergence of intermediates such as *COOH, *CHO, *OCH 3 , etc ., and elucidate the mechanism accordingly. This research contributes to the advancement of photocatalytic CO 2 RR, offering insights into applying Ti 3 C 2 Tx MXene in photocatalysis.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Yisha Zheng,Shuoling Lei,Wenjie Guo,Wenlong Xiang,Yanmei Chen,Yanhui Zhang
The high toxicity and persistence of nitroaromatic pollutants pose a serious threat to aquatic ecosystems. In this study, inert SiO 2 was employed as an "inactive enhancer" to construct core-shell MIL-125-NH 2 @ZIF-67/SiO 2 (M@Z/SiO 2 ) heterogeneous MOF catalysts via an epitaxial-wet impregnation method, enabling the efficient reduction of p -nitrophenol ( p -NP) under ambient temperature and pressure. Although SiO 2 itself lacks catalytic activity, the micro-mesoporous network it forms effectively disperses Co active sites and prevents their aggregation. The conversion rate of p -NP increased from 92.5% to 98.4% within 6 min and retained 98% activity after three consecutive cycles. Moreover, the catalyst exhibited excellent stability across a wide pH range (3-11) and in various anionic environments. Mechanistic studies revealed that the interfacial electron transfer between ZIF-67 and MIL-125-NH 2 significantly reduces the activation energy barrier of NaBH 4 . Additionally, the incorporation of SiO 2 not only enhances the mechanical stability of the composite but also optimizes pore structure and substrate mass transfer by modulating surface hydrophilicity. This work provides valuable insights for the precise design of MOF-on-MOF heterostructures and the synergistic engineering of interfacial and surface properties in environmental catalytic materials.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2025
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IF 6.3
Huihua Wang,Jinhong Wu,Siwei Guo,Haosen Chen,Ruiqi Guo,Ding Huan,Deyong Wang,Wenchang Li,Xianglong Li,Dong Hou
Engineering interface, regulating morphology, and doping heteroatoms are regarded as effective strategies for boosting the electrocatalytic performances of transition-metal phosphides (TMPs), while still encounter some challenges to obtain desirable stability and sustaining catalytic activity. Herein, the Fe-CoP/Ni 2 P@NC/CC-350 self-supported electrode was successfully synthesized via pyrolysis of FeNi/ZIF-67/CC precursors followed by phosphating. In this structure, Fe-doped CoP and Ni 2 P composite nanoparticles are uniformly confined in the porous carbon matrix and anchored firmly on the surface of carbon cloth (CC). Moreover, the flocculent-like Fe-CoP/Ni 2 P@NC/CC-350 demonstrates superhydrophilicity to significantly facilitate mass transfer, while the unique morphology originates from a facile strategy of soaking ZIF-67/CC in the mixed solution composed of FeSO 4 and NiSO 4 . The synthesized Fe-CoP/Ni 2 P@NC/CC-350 integrates the advantages of abundant active sites, confinement effect, interface regulation and superhydrophilicity, thereby demonstrating superior HER and OER activities and stabilities in an alkaline medium (1.0 M KOH). Remarkably, Fe-CoP/Ni 2 P@NC/CC-350 electrodes used both as anode and cathode require a cell voltage of only 1.49 V at 10 mA cm −2 , much lower than that of the well-established 20 % Pt-C/CC and RuO 2 /CC couple (1.612 V). Besides, Fe-CoP/Ni 2 P@NC/CC-350 Fe-CoP/Ni 2 P@NC/CC-350 system exhibits an outstanding stability for monitoring water splitting up to 100 h at 10 mA cm −2 . DFT results further confirm that the heterointerface and Fe doping in Fe-CoP/Ni 2 P@NC/CC-350 lead to a upshift d-band center of active sites and decreased reaction Gibbs energy barrier for the rate-determining step during catalysis, thereby contributing to the superior HER and OER activities. The work provides a novel strategy to construct a superhydrophilic microstructure, and the synergistic effect of electrons originating from the heterointerface and doping paves the way for designing electrocatalysts with high activities toward water splitting.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Rui Gou,Yong Li,Qilong Chen,Sha Wang,Dan Sun,Changhua Li,Xianmin Gong,Yi He
Metal corrosion causes a lot of waste of resources, and the protection of metals from corrosion is becoming increasingly important. In this study, zeolite-imidazole (ZIF-67) was grown on the surface of Co-MOF for the first time by a one-step (complexation) method. 2-Mercaptobenzimidazole (MBI) was then loaded into the inner cavity of ZIF-67, resulting in the formation of a new composite material, Co-MOF@ZIF-67@MBI. The modified Co-MOF exhibits excellent interfacial compatibility with the water-based epoxy resin, and the Co-MOF@ZIF-67@MBI composite coating demonstrates robust anti-corrosion properties. Following a 60-day immersion period, the electrochemical experiment demonstrated that the corrosion resistance modulus of the Co-MOF@ZIF-67@MBI composite coating reached 10 8 Ω cm², indicating that the coating effectively enhanced the corrosion resistance of the coating and significantly extended the service life of the coating.
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高影响因子
International Journal of Electrochemical Science
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2024
·
IF 1.3
Jiang Pei,Wang Haibo,Fan Chenli,Zhang Xiaomi,Huo Tiantian,Xu Yiwei
A novel electrochemical sensor modified by aspartic acid polymer and carbonized-ZIF-67 was prepared for arbutin detection. ZIF-67 was synthesized and carbonized, and then used as the substrate supporting of electrochemical sensor. Carbonized-ZIF-67 had a large specific surface and good electrical conductivity, which provided large electroactive area and promoted the electron transfer at the sensing interface. Aspartic acid polymer was prepared by cyclic voltammetry. Aspartic acid polymer could effectively absorb arbutin, resulting in the preconcentration of arbutin on sensor surface. Benefiting from the synergistic effect between carbonized-ZIF-67 and aspartic acid polymer, the prepared electrochemical sensor exhibited sensitive electrochemical response for arbutin. Under the optimum conditions, the electrochemical sensor achieved a wide linear range in the range from 5 to 110 μmol/L and a low detection limit of 0.41 μmol/L for arbutin. In practical application, the electrochemical sensor was employed to detect arbutin in green tea and whitening cream samples, exhibiting satisfactory recovery rates. With the outstanding features of easy operation, rapid response and high sensitivity, the prepared electrochemical sensor provided a convenient and effective tool for arbutin detection.
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高影响因子
ACS Applied Materials & Interfaces
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2024
·
IF 8.3
Deshuang Lu,Nikom Klomkliang,Francis Verpoort,Somboon Chaemchuen
Tailor-made unsaturated coordination of metal ions or organic linkers in zeolitic imidazole frameworks (ZIFs) has great potential in tuning the ZIFs’ properties and reactivity for their applications. Taking advantage of the solid-state thermal (SST) method as a facile and eco-friendly synthesis method, the rational coordination of metal ions with imidazole ligands in ZIF-67 through the SST method is investigated. The rational precursor ratio (metal-to-ligand source) under the solvent-free SST method emerges as a perfect strategy to tune the coordinately unsaturated sites within the ZIF-67 frameworks. Different analysis techniques, computational methods (DFT), and catalytic model reactions examine unsaturated coordination in ZIF-67 materials (defect structures). The unsaturated coordination provides unique characteristic properties on materials with excellent catalytic performance. However, the higher reactive properties are negotiated with weaker structural stability on materials. In addition, the post-SST approach is applied to enable rational coordination and modify the pristine ZIF-67 materials. The post-SST method rearranges and modifies coordination in the framework of materials. These findings are crucial to understanding the role of the uncoordinated degree to balance with structural stability based on ZIF-67, which is critical for effective heterogeneous catalysts.
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PubMed
高影响因子
DESALINATION
·
2025
·
IF 9.8
Yifan Shao,Chao Hu,Ruirui Liu,Bingxin Liu,Yongquan Zhou,Jianming Pan
The design of adsorbents with high recognition activity, high site density and high mass transfer efficiency is the significant to the removal of specific non-metallic ions from Salt Lake brines. Here we report the fabrication of ZIF-67-derived hollow Co 3 S 4 nanoadsorbent for the adsorption and separation of boron (B) in complex water from concentrated salt solutions. The adsorption experiments displayed that the B adsorption capacity of the hollow Co 3 S 4 material exhibited substantial B adsorption capacity, reaching 283.3 mg·g −1 , which represents an impressive 7.3-fold improvement over ZIF-67. On these grounds, a series of kinetic and thermodynamic studies were conducted, and the results revealed that the adsorption process is more consistent with the spontaneous exothermic reaction of the Langmuir adsorption isothermal model (R 2 = 0.999). The results of the charge density and density of states depicted that Co atoms strongly interact before and after adsorption, and that Co atoms are tend to react spontaneously with H 3 BO 3 , which serves as the primary adsorption site. The interaction including electrostatic and hydrogen bonds jointly realizes in B adsorption performance with high selectivity and excellent cycle stability. This study highlighted the high adsorption performance of the hollow Co 3 S 4 for boron in real water of the Salt Lake brine and provided a new idea for the design of other ZIFs derived hollow nanoadsorbent for practical applications.
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高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2025
·
IF 4.1
Run Cai,Jiahao Jiang,Pengfei Diao,Zihan Wei,Change Yao,Bosheng Zhou,Huijuan Zhang,Wenwen Liu,Zhong Ma
It is crucial to develop low-cost and efficient electrocatalysts to facilitate oxygen reduction reaction (ORR) and transition metals incorporated into nitrogen-doped carbon matrices (M-NC) catalysts are regarded as a potential candidate to substitute platinum-based electrocatalyst. However, there is still a great challenge in real activity and stability, compared to Pt-based electrocatalysts, for large-scale applications. An effective way to improve the ORR performance for this category of single-atom catalysts is to increase the density of active sites. In this work, therefore, the highly dispersed ZIF-67-derived Co-NC confined in carbon pores electrocatalysts are synthesized by impregnating ZIF-67 precursors into the nanopores of Ketjenblack EC-600JD (KB) resulting in the in-situ growing of small crystals in the pores followed by the high temperature pyrolysis. The as-prepared CoNC-700@C electrocatalyst exhibits excellent ORR performance in alkaline media with an onset potential of 967 mV and a half-wave potential of 892 mV (vs. RHE), which is much higher than that of the commercial Pt/C catalyst. It is inferred that the excellent ORR activity of CoNC-700@C mainly results from the increased density and also enhanced dispersion of active sites due to the confinement effect offered by the pores of KB. This study also provides a simple and effective method to increase the density of active sites for single-atom category materials.
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高影响因子
Advanced Composites and Hybrid Materials
·
2022
·Vol. 5
·期 4
·2988-3001
·
IF 11.806
Zhao Xiaoyu,Zhang Yingbing,Hou Yongdan,Zhao Zijian,Gong Yaxin,Wang Yanfei,Wei Huige,Pol Vilas G.
A beneficial strategy for enhancing the electronic conductivity of transition metal chalcogenides (TMCs) as lithium-ion battery anode material is through shortening the charge transfer path between the sulfide particles. However, the combination between the carbon-based matrix and electroactive materials is sometimes weak, which hinders the cycling stability. In this paper, the Ti-based MXene, T 3 C 2 T x , was used as a conductive frame, combined with the ZIF-67-based CoS 2 /C grains yielding Ti 3 C 2 T x /CoS 2 /C composite electrode through one-step and two-step synthesis methods, which displayed significantly enhanced capacity, rate performancem, and cycling stability. The compsoite reached a capacity retention of 82.6% after 100 cycles with a significantly higher capacity of 1020.5 mAh/g at 0.2 A/g current density. After 100 discharge–charge cycles, the Ti 3 C 2 T x /CoS 2 /C composite revealed a low volume expansion of 9.5%, suggesting superior structural integrity and stability with the synergistic effect of both MXene 2D and CoS 2 /C 3D nanostructures. Graphical abstract
研究领域:
材料科学
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电化学
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能源存储
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高影响因子
危险品化学品经营许可证（带存储）