ChemCatChem
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2016
·Vol. 8
·期 6
·1111-1118
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IF 4.724
Xinlin Li,Wei Zhang,Yansheng Liu,Rong Li
Graphical Magnetic personality : A new magnetic porous carbon derived from metal–organic framework is synthesized through the direct carbonization of ZIF-67 crystals and utilized as a support for Pd nanocatalysts. The catalysts are tested in the semihydrogenation of phenylacetylene under extremely mild conditions. A new magnetic porous carbon (MDPC) derived from metal–organic frameworks (MOFs) was synthesized successfully through the direct carbonization of ZIF-67 crystals and utilized as a support for Pd nanocatalysts. The prepared MDPC not only retains the original morphology of ZIF-67 crystals but also provides a high surface area and excellent magnetic properties. The designed catalysts (Pd-MDPC) were tested in the semihydrogenation of phenylacetylene under extremely mild conditions. The Pd nanoparticles are highly dispersed on the MDPC matrix without aggregation and exhibited an excellent catalytic activity and high selectivity toward olefins under mild conditions (25 °C, H 2 1 atm). The Pd-MDPC catalysts were further investigated in the semihydrogenation of several other terminal alkynes. Compared with most traditional carbon materials, such as activated carbon and carbon nanotubes, the MDPC possesses an admirable magnetism so that it could be separated magnetically from the reaction system. Our study indicates that MOF-derived porous carbon is a suitable support for noble-metal nanocatalysts and has promise in the field of nanocatalysis.
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Journal of Environmental Chemical Engineering
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2024
·
IF 7.4
Longfei Qiao,Yu Shu,Yan Gao,Hua Fan,Jiaqing Zhao,Jingjing Zhang,Hiroshi Uyama,Yehua Shen
The physical properties and chemical compositions of porous carbons are crucial factors in determining their effectiveness in adsorbing CO 2 . Cellulose-based porous carbon has emerged as an outstanding candidate adsorbent for CO 2 capture. The research involved the creation of hierarchically nitrogen-doped porous carbon (HNC) using a 3D cellulose alcogel (CA) as substrate, which was prepared through a thermal introduced phase separation (TIPS) method combined with hydrolysis treatment. The plentiful functional groups of CA offered abundant growth sites for the introduction of ZIF-8 crystals. CA/ZIF-8 composite alcogel (CZA) with greater surface area and superior thermal stability compared to CA was successfully fabricated and used as precursor for the production of HNC. The important effects of microporosity and surface chemistry of HNC samples on CO 2 capture were discussed in-depth. HNC-350–850 displayed a hierarchically porous structure with a large number of micropores and abundant N/O/Zn-doped functional groups, exhibiting high CO 2 uptakes at 1 bar (3.56 mmol/g at 25 °C), good IAST CO 2 /N 2 (15/85, V/V) selectivity of 16.31 at 25 °C, and outstanding regenerability with ∼100 % CO 2 adsorption capacity retained after ten cycles. In the two-component CO 2 /N 2 (15/85, V/V) competitive adsorption process, the maximum breakthrough periods for CO 2 (433.1 s) is significantly longer than that of N 2 (3.8 s). The CO 2 breakthrough adsorption capacity reached 1.79 mmol/g at 25 °C and 1 bar with the separation coefficient of 45.8 for CO 2 over N 2 . These results confirmed that HNC, in addition to having excellent CO 2 /N 2 selectivity, demonstrated good feasibility for practical use. The green and practicable synthetic route described in this study is not only expected to offer novel adsorbents for high performance CO 2 capture, but also provide a new theoretical foundation for the development of cellulose-based porous materials.
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FOOD CHEMISTRY
·
2025
·
IF 9.8
Zi-Ling Li,Xiao-Run Qi,Yi-Heng Xu,Jia-Qi Zhao,Gui-Fu Zuo,Man-Man Wang
Effective and convenient QuEChERS of lipophilic pesticides with wide p K a range from strongly pigment-rich food samples remains a great challenge. Here, ZIF-67 derived magnetic nanoporous carbon (Co@MPC) was firstly proposed for modified QuEChERS of carbamate pesticides ( pK a 4.3–12.3) in various vegetable and fruit samples prior to LC-MS/MS. This sorbent offered superior adsorption capacities of 29.89 mg/g and 22.28 mg/g towards chlorophyll and lutein via π-π and hydrophobic interactions. The present method exhibited acceptable matrix effect of −4.8 %-14.4 %, low detection limits of 0.003–0.02 μg/kg and satisfactory recoveries of 80.2 %–108 % in celery, cabbage, Chinese cabbage, apple, banana and orange samples. 10 mg of Co@MPC enabled highly efficient matrix purification and isolation in 20 s, offering low-cost and facile clean-up process. The study highlighted great potential of Co@MPC as QuEChERS sorbent, and demonstrated its wide applicability and broad application prospects to monitor the contaminants in food items.
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PubMed
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Shouwu Xu,Zhilong Zhang,Hailin Zhang,Zhiwei Li,Haoping Peng,Sibudjing Kawi,Aijun Xie,Ping Qiu
The development of a photoelectrochemical cathodic protection film with electron storage capabilities offers a feasible method for metal protection in the absence of light. In this study, we designed and fabricated an innovative TiO 2 /ZIF-67 composite film in situ. The synthesized ZIF-67 nanoparticles with a dodecahedral structure not only facilitate contact with the electrolyte but also significantly broaden the sunlight absorption range. When coupled with 304 SS, the TiO 2 /ZIF-67-20 composite film demonstrated a minimum OCP value of −0.675 V (vs. SCE) under illumination. Notably, even after 10 h of light deprivation, the OCP remained lower than that of 304 SS. This sustained protection can be attributed to the electronic storage and release capabilities of the Co element within the TiO 2 /ZIF-67 composite, ensuring continuous cathodic protection for 304 SS during both illuminated and dark conditions. This study contributes valuable insights into achieving all-weather cathodic protection for 304 SS.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
·
IF 4.9
Gongheng Zhang,Abdullah Ali Mohammed Ahmed Al-Anzah,Fengxiang Yin,Jie Zhang,Guoru Li,Biaohua Chen,Qiuyue Gao,Xian Tong Yu,Yuqian Sun
The precursor ZIF-67/xC-T was prepared by solvothermal and pyrolysis methods. A series of ZIF-67/xC-T-yIL catalysts were then prepared by modifying the surface of the precursor with [BMIM][NTf 2 ] ionic liquid . The results showed that [BMIM][NTf 2 ] as sulfur and nitrogen sources, N, S co-doped carbon can improve the catalytic activity of ORR . Meanwhile, [BMIM][NTf 2 ] formed an oxygen-rich layer on the catalyst surface, which increased the contact between oxygen and the active sites, reduced the alkaline strength of the catalyst surface, and improved the desorption ability of the catalyst to the product. Therefore, the ZIF-67/xC-T-yIL catalyst exhibited better ORR activity in an alkaline electrolyte than the catalyst without [BMIM][NTf 2 ]. Among the ZIF-67/xC-T-yIL catalysts, ZIF-67/1.2 C-600–6IL demonstrated the best ORR catalytic activity, with a half-wave potential of 0.86 V and a limiting current density of 5.21 mA cm −2 in 0.1 mol L −1 KOH, which was comparable to that of commercial 20% wt% Pt/C.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Zhongming Zhang,Enfang Gou,Zhiying Zhao,Rui Wu,Rui Fang,Weipeng Guo,Jie Yao
Organophilic pervaporation (PV) mixed matrix membranes (MMMs) have enormous potential for organic wastewater treatment due to their environmental friendliness and high efficiency. However, developing a high-flux PV membrane remains challenging. In this work, the nanocage-like hollow ZIF-71(h) (HZIF-71(h)) polyhedral nanocrystals were synthesized by heteroepitaxial growth of a ZIF-71(h) shell and successive excavation of a ZIF-67 core. The resultant HZIF-71(h) nanocrystals were blended with poly (ether block amide) (PEBA) matrix to fabricate MMMs for phenol/water separation. Results from several characterization techniques confirmed the successful preparation and formation mechanism of HZIF-71(h). Further, a series of experiments were conducted using the composite membranes to explore the impact of filler type, filler loading, operating temperature, and feed concentration on the separation performance. The incorporation of ZIFs facilitated phenol permeation while limited water transport, thereby resulting in increased separation factor. Notably, the HZIF-71(h)/PEBA-21 MMM exhibits a higher phenol flux in comparison to ZIF-71/PEBA-21 and ZIF-67/PEBA-21 MMMs, indicating the importance of the low-resistance hollow structure. The HZIF-71(h)/PEBA-21 MMM exhibits outstanding pervaporation performance with a separation factor of 15.86 and a phenol flux of 17.32 g·m −2 ·h −1 , respectively, displaying an improvement of 41.2 % and 6.4 % compared to the PEBA/PVDF membrane. Furthermore, this composite membrane demonstrated outstanding durability during continuous testing for 84 h, implying a promising potential for phenol separation.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Feiyu Gao,Chaowen Tan,Yang You,Yong Hou,Hongyan Yan,Xuewei Lv,Jie Dang
The imperative need for efficient and selective adsorption of Ni(II) and Mo(VI) is crucial for resource utilization and environmental protection. However, this process faces a challenge due to the scarcity of adsorbents that can adeptly adsorb both metal ions simultaneously. To address this, this study introduces a novel composite adsorbent material, denoted as BECZN, achieved through composite cross-linking of waste orange peel biochar with in situ aminated cobalt/zinc-zeolitic imidazolate frameworks (Co/Zn-ZIF-NH 2 ). The incorporation of Co/Zn-ZIF-NH 2 enhances the availability of active groups within BECZN. The aerogel structure of BECZN prevents ZIF material collapse and agglomeration, thereby improving active site exposure. BECZN exhibits notable adsorption capacities, reaching 151.84 mg/g for Ni(II) at pH = 7 and 842.54 mg/g for Mo(VI) at pH = 3. Further investigations indicated that the adsorption of Ni(II) and Mo(VI) obeys the Langmuir isotherm model, while exhibiting pseudo-second-order kinetics and intraparticle diffusion characteristics. Notably, BECZN selectively adsorbs Ni(II) and Mo(VI) efficiently under acidic and neutral conditions, respectively. It can maintain high capacity under the interference of various cations and anions. Meanwhile, this excellent selective adsorption of Ni(II) and Mo(VI) by Co/Zn-ZIF-NH 2 is revealed at the atomic level using density functional theory (DFT) calculations. This study offers a theoretical basis and experimental reference for the design and synthesis of ZIF and biomass-based composite adsorbents.
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CERAMICS INTERNATIONAL
·
2024
·
IF 5.1
Jiasheng Fang,Zhenting Huang,Ming Chen,Shuo Zhao,Zhihui Liang,Qiongfang Zhuo,Yongfu Qiu
The utilization of natural clay minerals for synthesizing nano-sized metal-organic frameworks (MOFs) supported materials offers great advantages for rational design of innovative catalysts, which promotes the low-cost and large-scale environmental remediation applications. This work reported a facile and scalable encapsulation-pyrolysis strategy to prepare novel Au-HNTs@Co-NC core-shell catalyst for catalytic reduction of nitroaromatic pollutants. The HNTs were modified with aminosilane on the external surface for effectively anchoring well-dispersed and ultrasmall Au NPs. Uniform nano-sized ZIF-67 crystals controllably embraced the Au-HNTs via in-situ growth induced by electrostatic adsorption. The N 2 atmosphere pyrolysis at 550 °C resulted in Co NPs embedded into N-doped carbon substrates, and transformed ZIF-67 crystals into Co-NC layers for preferable encapsulation and stabilization of Au NPs. The as-prepared Au-HNTs@Co-NC-550 catalyst manifested splendid catalytic performance for p-nitrophenol reduction, and achieved the reaction rate constant and TOF value estimated as 2.025 min −1 and 49.25 min −1 , which significantly exceeded the behaviors of as-prepared control materials. Moreover, the catalyst also displayed excellent catalytic capability toward the reduction of nitroanilines and homologues and isomers of p-nitrophenol, indicative of its decent general applicability. After 8 cycles of reactions, the catalyst still retained brilliant reusability and structural stability with good magnetic property for expedient separation. The advantageous hollow core-shell structure combining HNTs and ZIF-67 derivatives enhanced the reactant diffusion and transfer. The N doping and electronegativity difference between Co and Au aroused higher electron uptake and facilitated electron transport during the reduction process. Meanwhile, the Co–H and Au–H bonds formed the strong synergistic effect for superior cooperative catalytic performance of the catalyst.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2024
·
IF 4.1
Haopeng Gao,Kangming Wang,Xiangyu He,De Li,Cheng Zheng,Yong Chen
Dual-ion batteries (DIB) have drawn much attention because of their advantages such as low cost, high energy density, and high power density. Graphite has been considered as one of the most promising cathode materials for DIBs due to its low cost, good electron conductivity, environment friendliness and unique two-dimensional layered structure. However, graphite still suffers from limited cycling stability caused by the structural collapse of graphite, resulting from the repeated intercalation/deintercalation of anions, solvent co-intercalation, and electrolyte decomposition on the electrode/electrolyte interface. In this work, the electrochemical performances of graphite cathode are significantly enhanced through a simple way by in-situ coating of the hydrolysate Zn 5 (HMIM) 4 (MIM) 6 (OH) 4 (labeled as ZnHM) derived from ZIF-8, which was performed in aqueous solution at room temperature. It is found that a capacity retention as high as 84 % with the discharge capacity of 65 mA h g −1 after 1000 cycles at 100 mA g −1 was achieved. More importantly, ca. 70 % of the initial discharge capacity is retained even after 3000 cycles at 500 mA g −1 . These remarkable electrochemical properties are attributed to the coating layers of ZnHM on graphite surface, which inhibit the co-intercalation of solvent molecules, keep the structural stability of graphite, and hinder the decomposition of electrolyte.
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TALANTA
·
2024
·
IF 5.6
Yaqin Zhan,Jinru Cao,Ying Wang,Xuesong Li,Yixing Li,Huihui Zeng,Wenyi Huang,Hao Cheng,Si Gao,Lijun Li,Jun Feng
Surface Enhanced Raman Scattering (SERS) has been extensively utilized in therapeutic drug monitoring (TDM) due to its rapid detection speed, high sensitivity and straightforward sample pretreatment. In this study, Au/AgNPs were obtained through the reduction of AgNO 3 on the surface of AuNPs. Subsequently, Au/AgNPs were embedded into the tetrahedral lattice of ZIF-8 MOFs, resulting in the formation of Au/Ag@ZIF-8 nanocomposites. The Au/Ag@ZIF-8 nanocomposites exhibit a robust electromagnetic enhancement of Au/Ag bimetallic nanoparticles and a considerable adsorption capacity of ZIF-8 MOFs. This enables the pre-enrichment of target molecules in the vicinity of the electromagnetic field of the Au/AgNPs, thereby enhancing the sensitivity of SERS detection. The SERS substrate also exhibits high stability and reproducibility, as well as molecular sieving effects, due to the fact that Au/AgNPs are embedded into the tetrahedral lattice of ZIF-8. A TDM method for tacrolimus (FK506) in human serum was developed by using Au/Ag@ZIF-8 nanocomposites as solid phase extraction (SPE) adsorbent and SERS substrates. The results showed that under the optimized conditions, tacrolimus exhibited satisfactory linearity within the concentration range of 10 −5 -10 −11 mol L −1 , with a correlation coefficient (R 2 ) of 0.9944, and the limit of detection (LOD) was as low as 6.4 pg mL −1 . The recoveries were observed to range between 92 % and 105 %, with an RSD of below 8 %. The method is highly sensitive, exhibiting a sensitivity that is 3-6 orders of magnitude higher than that of existing analytical techniques. It has the potential to be applied in a clinical setting to biological samples.
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ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Bin Jiang,Congcong Zhang,Na Yang,Qi Zhou,Longfei Zhang,Jingshuai Li,Wei Yang,Xiaodong Yang,Luhong Zhang
Developing highly active photocatalysts that can directly utilize clean, cheap, and sustainable solar energy to achieve an efficient carbon dioxide (CO2) cycloaddition reaction under mild reaction conditions (1 bar of CO2) remains a great challenge. In this paper, 2D/2D ZnIn2S4/Zn-NC S-scheme heterojunction composites were constructed by the in situ growth of layered ZnIn2S4 on the surface of two-dimensional (2D) ZIF-L-derived Znδ+ (0 ≤ δ ≤ 2) and N codoped carbon skeletons (Zn-NC-T) via a low-temperature solvothermal method. The optimized ZnIn2S4/Zn-NC-T photocatalysts exhibited favorable photocatalytic CO2 cycloaddition performance, and the yield of cyclic carbonate reached about 98.8% under 10 mmol epoxides reactant, 1 bar CO2 pressure, and full-spectrum irradiation for 4 h. The favorable photocatalytic performance is attributed to the efficient photothermal conversion and effective separation of photogenerated carriers induced by the carbon matrix and heterojunctions, respectively. In addition, the stability of the heterojunction structure and activity were demonstrated through cyclic experiments. Furthermore, the possible mechanism of S-scheme heterojunction photocatalytic CO2 cycloaddition is proposed through electron paramagnetic resonance (EPR) spectra, cyclic voltammetry (CV) experiments, and quenching experiments. The mechanism analysis proved that light irradiation is conducive to the transfer of photogenerated electrons from the conduction band of ZnIn2S4 to epoxides, promoting the formation of ring-opening intermediates, and photogenerated holes may promote the coordination and polarization of adsorbed epoxides. This work not only prepared an S-scheme heterojunction catalyst with excellent photocatalytic CO2 cycloaddition performance but also provided new insights for the rational design of heterojunction catalysts for photocatalytic CO2 cycloaddition.
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ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Rui Wang,Yixin Yan,Lu Wang,Xiaoya Kang,Shengtao Niu,Youzhi Wu,Fen Ran
Metal-organic framework draws widespread interest on account of its large specific surface areas, which could be employed as sacrificial templates to synthesize Co/N-doped carbon nanocubes. Herein, Ni-Co 3 ZnC is used as an additive for improving the electrical conductivity as well as lithium-storage performance of Co/N-doped carbon because of the conductivity and catalytic activity of metal nanoparticles . Co/N-doped carbon nanocubes and Co/N-doped carbon-Ni-Co 3 ZnC anode materials are prepared through one-step precipitation and high-temperature calcination methods. The lithium-storage capabilities of Co/N-doped carbon and Co/N-doped carbon-Ni-Co 3 ZnC are investigated. Co/N-doped carbon-Ni-Co 3 ZnC manifests good electrochemical performance at 2.0 A g −1 compared to Co/N-doped carbon. The initial reversible capacities of Co/N-doped carbon and Co/N-doped carbon-Ni-Co 3 ZnC are 877.4/548.4 and 1, 170.5/557.3 mAh g −1 , and the reversible capacities could be maintained at 152.6/152.4 and 276.8/276.5 mAh g −1 after 2, 000 cycles. The electrode kinetic results evidence that Ni-Co 3 ZnC could enhance the conductivity of Co/N-doped carbon. The data provide a theoretical basis for improving the lithium-storage performance of prevalent anode materials.
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