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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2023 · IF 7.2

Optimizing electrocatalytic hydrogen evolution performance of derived materials by using organic ligands containing sulfur elements for Co-MOF

Ling Qin,Xiao-Yan Zhou,Ying-Xin Zhao,Jin-Long An,Jing-Yu Huang,Wang-Chao Chen,Ming-Dao Zhang

The rational preparation and development of efficient and stable non-precious metal catalysts for the hydrogen evolution reaction are an effective solution to solve the global energy shortage and the increasing environmental pollution problems. Herein, two Co-MOFs with similar structures were designed and synthesized, one based on sulfur-containing organic ligand and the other based on non-sulfur-containing organic ligand. The electrocatalytic performance results showed that the materials based on sulfur-containing organic ligand had a better electrocatalytic hydrogen evolution performance. The reasons of performance differentiation were analyzed by various characterization techniques.

CAS / MDL: 10026-22-9
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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

A versatile MOF liquids-based Janus fibrous membrane towards complex oil/water separation and heavy metal ions removal

Bingbing Cheng,Xinming Fu,Yiheng Song,Zehao Li,Puxin Weng,Xianze Yin

As an emerging material, porous liquids (PLs) have attracted wide attention and are applied in oily wastewater for the effective elimination of heavy metal ions due to their permanent pore structure, mobility, and superhydrophilicity. However, it remains a challenge to further enhance the separation performance of PLs. Here, a novel metal–organic framework (MOF) porous liquid was synthesized and mixed with a polyacrylonitrile (PAN) solution to produce an asymmetrical Janus fibrous membrane by electrostatic spinning technique. Benefiting from the synergistic effect of the electric field and self-migrating properties of MOF PLs, the Janus membranes exhibited ultrahigh flux of 25310.26 L m -2 h −1 bar −1 , outstanding separation efficiency (reaching up to 99.99 %) in various oil–water emulsions and high antimicrobial activity (>99.9 %). More impressively, the obtained Janus membranes maintained long-term stability, with separation efficiencies consistently as high as 99.5 %. Meanwhile, the porous structure of MOF PLs with abundant active sites and affinity of polyethylene glycol (PEG) flexible chain for metal ions facilitates the adsorption of metal ions with a maximum equilibrium adsorption capacity of 205 mg/g, which is superior to other literature reported. These results demonstrated that the versatile MOF PLs-based Janus fibrous membranes had a promising application prospect in addressing the challenges associated with such wastewater treatment.

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JOURNAL OF ALLOYS AND COMPOUNDS · 2023 · IF 6.2

Bayberry-like bimetallic CoNi-MOF-74 derivatives/MXene hybrids with abundant heterointerfaces toward high-efficiency electromagnetic wave absorption

Tong Wu,Fang Ren,Zhengzheng Guo,Jiale Zhang,Xin Hou,Zhengyan Chen,Yanling Jin,Penggang Ren

The flourishing development of electronic devices and radar detection technologies necessitates the urgent creation of high-efficiency electromagnetic wave (EMW) absorption materials with expansive absorption bandwidths. Although MXene has garnered significant interest in the domain of EMW absorption due to its tunable dielectric properties and structural designability, its high permittivity often results in poor impedance matching and a single loss mechanism, which makes it difficult to realize optimal EMW absorption capabilities. In this work, CoNi bimetallic metal–organic frameworks (MOFs) derived bayberry-like magnetic porous carbon (CoNiMPC)@carbon nanotubes (CNTs)/MXene (CNCM) hybrids were initially synthesized via simple solution precipitation, thermal treatment, and electrostatic self-assembly strategy. As anticipated, excellent EMW absorption characteristics were achieved by adjusting the ratio of CoNiMPC@CNTs and MXene. Multi-heterointerfaces consisting of zero-dimensional porous carbon , one-dimensional carbon nanotubes, and two-dimensional (2D) MXene, electrical/magnetic coupling effects, and polarization loss induced by abundant heterointerfaces endow the prepared CNCM hybrids with high-performance EMW absorption. Notably, the CNCM-7 hybrid material exhibits a minimum reflection loss (RL min ) of − 65.3 dB at 6.8 GHz with a mere 2.7 mm thickness and an effective absorption bandwidth (EAB, RL < −10 dB) of 5.0 GHz at a thickness of 1.27 mm. This study proposes a unique viewpoint and approach towards the design and preparing high-performance MXene-based EMW absorption materials.

CAS / MDL: 7789-24-4 693-98-1
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Environmental Technology & Innovation · 2023 · IF 7.1

MOF-based Ca-alginate/PAA granulate beads for efficient heavy metal removal from water: Synthesis, performance, and mechanism

Tengfei Wu,Junjie Lei,Liyun Lin,Qing Wang,Taimoor Hassan Farooq,Guangjun Wang,Jun Wang,Wende Yan

Developing high-efficient and easy-to-recover adsorbents for the removal of toxic metals in water is imperative, although it poses a huge challenge. In this study, a sulfur-functionalized metal-organic framework was incorporated into Ca-alginate/polyacrylic acid granulates as an effective adsorbent ( abbr. CPZ-SH) for Cu 2+ and Cd 2+ removal. The physicochemical properties of the obtained CPZ-SH were determined by the integrated characterization techniques (e.g., FTIR, XRD, and SEM). The environmental effects of solution pH, typical background cations (K + , Na + , Mg 2+ , and Ca 2+ ), and dissolved organic matter were assessed to determine the adsorption behaviors of the granulates. Time-dependent adsorption kinetics suggested that the adsorption process was dominated by an intraparticle diffusion procedure. CPZ-SH exhibited maximum adsorption capacities of 75.8 and 48.4 mg g –1 at 30 ℃, and excellent adsorption reusability with Cu 2+ and Cd 2+ adsorption efficiencies over 96.0% and 85.1% after 10 cycles, respectively. The extended X-ray absorption fine structure (EXAFS) demonstrated that the functional groups (thiol, carboxyl, and hydroxyl) played a crucial role in adsorption processes. The findings provided an effective strategy to construct nanostructured metal-organic frameworks (MOFs) into granulates as recyclable adsorbents and enable heavy metal removal from water.

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ACS Applied Nano Materials · 2023 · IF 5.9

Metal–Organic Framework (MOF)-Based Single-Atom Iron Catalysts for NIR-II Enhanced Catalytic-Photothermal Synergistic Antibacterial Therapy

Changrui Ying,Xiaolong Zhu,Shuqing Xiang,Mingqian Wang,Xuefeng Jiang,Jian Shen

Single-atom catalysts based on carbon-based materials have a high catalytic activity and excellent photothermal performance. In this article, iron single-atom catalysts loaded on C-MOF-5 carriers have been prepared for the application of photothermal catalytic antimicrobial therapy. Iron single-atom catalysts (Fe SACs) exhibit significant peroxidase-like catalytic activity and catalyze the production of large amounts of hydroxyl radicals (·OH) when hydrogen peroxide is present, which have a killing effect on bacteria. In addition, the excellent photothermal properties of the carbon material allow Fe SACs to rapidly generate a localized high temperature under NIR-II laser light (1064 nm) to kill bacteria and enhance peroxidase-like catalytic activity to produce a large number of hydroxyl radicals. In vitro bacterial assays demonstrated that the synergistic antimicrobial strategy of chemodynamic therapy (CDT) and photothermal therapy (PTT) is nearly 100% effective against E. coli and S. aureus, demonstrating greater antimicrobial efficiency than chemodynamic therapy and photothermal therapy alone. In vivo bacterial assay shows better wound healing in mice treated with CDT, PTT synergistic antimicrobial therapy. In summary, these carbon-based single-atom catalysts could be used as antimicrobial agents through the CDT and PTT synergistic antimicrobial effect.

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NANOTECHNOLOGY · 2023 ·Vol. 34 ·期 49 ·495102 · IF 3.5

Porous carbon nanosheets derived from two-dimensional Fe-MOF for simultaneous voltammetric sensing of dopamine and uric acid

Shouhui Chen,Dan Zhou,Jingguo Yu,Zhenzhong Huang,Li Wang

It is of great significance for electrochemical sensors to simultaneously detect dopamine (DA) and uric acid (UA) related to biological metabolism. In this work, two-dimensional (2D) porous carbon nanosheets (CNS) was prepared as electrocatalysts to improve the sensitivity, the selectivity, and the detection limit of the simultaneous detection. First, 2D amorphous iron-metal organic frameworks (Fe-MOF) was synthesized with Fe3+ and terephthalic acid via a facile wet chemistry method at room temperature. And then, CNS was prepared by pyrolysis and pickling of Fe-MOF. CNS had large specific surface area, good electrical conductivity and lots of carbon defects. The response currents of the CNS modified electrode was larger than those of the control electrodes in the simultaneous determination. The simultaneous determination was measured via differential pulse voltammetry to reduce the effect of capacitive currents on quantitative analysis. The CNS modified electrodes showed high sensitivity and low detection limit for the simultaneous detection of DA and UA. The modified electrodes have been successfully used to detect DA and UA in normal human serum.

CAS / MDL: 62-31-7 69-93-2 100-21-0
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Sustainable Energy & Fuels · 2023 ·Vol. 7 ·期 23 ·5557-5564 · IF 5.6

MOF-derived Fe–N–C electrocatalyst via a dual ligand strategy for efficient oxygen reduction in acidic media

Yi Sheng,Hongmei Zheng,Jingting Hou,Wanying Zhang,Hong Chen,Luanjie Nie,Jing Zheng,Qingxue Lai

Fe–N–C materials as popular non-Pt group metal (non-PGM) electrocatalysts demonstrated huge potential for replacing Pt-based materials for efficient oxygen reduction reaction (ORR) electrocatalysis in acidic media. Herein, a metal–organic-framework (MOF)-based dual ligand strategy is proposed to develop advanced Fe–N–C materials with a controllable density of Fe-Nx sites and electrochemically active surface area, attributed to the synergistic effect from secondary ligand manipulation and Zn evaporation during pyrolysis. As a result, the optimized catalyst exhibits an ORR half-wave potential of 0.747 V vs. RHE and long-term stability with only a 29 mV negative shift after 3000 potential cycles in 0.5 M H2SO4 electrolyte. More far-reaching, this MOF-based dual ligand strategy opens a novel avenue to the precise fabrication of efficient catalysts.

CAS / MDL: 10312-55-7
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

A 3D homogeneous microreactor with high mixing intensity at wide Re range for MOF preparation and POCT application

Zhongjian Tan,Huanhuan Shi,Yun Zheng,Yu Cao

Most microreactors can only work under high Re or extremely low Re conditions to obtain enough mixing efficiency, the inefficient reaction intensity undoubtedly limits its application scenarios. In this study, a novel 3D homogeneous microreactor (3D-HM) was reported that demonstrate a strong mixing intensity over a wide range of Re conditions. The 3D geometries of shunt and lateral secondary flow structure were optimized in details, and then were added to the Zigzag mixing channel to promote mixing index (MI) (over 94 % from Re  = 0–10, and more than 98 % for Re  > 10). Compared with the traditional T-shaped, Split and Recombine micromixer, a shorter mixing distance ( L mix ) and mixing time ( τ mix ) were needed to realize fully mixing. The 3D-HM was used for the preparation of Zeolitic imidazolate framework (ZIF-8), the particle size, yield and drug loading capacity of ZIF-8 prepared using the 3D-HM under a milder Re conditions were better than those prepared by traditional and existing microfluidic methods under a harsh Re conditions. The promotion to diffusion mixing with 3D-HM channel was then verified using the enzymatic catalytic reaction driven by syringe pump at low Re and capillary pump, respectively. Enzyme and substrates in the laminar flow in the 3D-HM are more likely to bind each other than that in the T-shaped diffusion mixing. In addition, the laminar diffusion mixing process was scaled up by microfluidic channel design, so that the results of enzymic catalytic reaction was visualized for Point-of-care Testing (POCT) application. The MI, L mix and τ mix directly determine the homogeneous microreaction intensity. The proposal of the 3D-HM may provide more possibilities for the application of micromixing-based reactors.

CAS / MDL: 5970-45-6
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2023 · IF 7.2

Accordion-like Co-MOF derived heterostructured Co/CoP@PNC as highly efficient electrocatalyst for alkaline hydrogen evolution reaction

Guoliang Gao,Dongwei Wei,Li Li,MingQi Wei,Xueli Chen,Yangyang Yu,Guang Yang,Guang Zhu,Lu Han,Jin Jia

Transition metal phosphates have proved to be promising electrocatalysts for hydrogen evolution reactions (HER) of water splitting, however, further increasing their active sites and catalytic activity remains a major challenge. Herein, accordion-like Co-MOF with layered structure was synthesized. After subsequent carbonization and phosphidization, lamellar heterostructured Co/CoP nanocrystals encapsulated in a P, N co-doped C matrix (Co/CoP@PNC) was obtained. Heterojunction provides abundant active sites and improves electron transfer rate. Additionally, the effect of phosphating degree on the electrocatalytic activity was studied. In the alkaline electrolyte , the current density of the optimized Co/CoP@PNC-10 for HER reached 10 mA cm −2  at overpotential of 137 mV in 1.0 M KOH, which was superior to most of transition metal-based electrocatalysts. This work provides new guidance for the design and development of transition metal-based electrocatalysts.

CAS / MDL: 67-56-1 7681-53-0
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Journal of Cleaner Production · 2023 · IF 11.1

Self-assembled TiO2/MOF on corrugated paper as a recyclable and efficient composite for dual-channel dye removal

Fan Luo,Min Li,Xianghui Liang,Jingxian Yang,Shuangfeng Wang,Xuenong Gao,Zhengguo Zhang,Yutang Fang

Adsorption separation and photocatalytic techniques have emerged as effective methods to eliminate organic dyes from water environment, but the poor recycling of most powdered adsorbents and photocatalysts in aqueous solutions hinders their commercial viability. Herein, we propose an effective and reusable dye-elimination module through the bottom-up self-assembly of photocatalyst (TiO 2 nanoparticles) and adsorbent (Al-fumarate) on a corrugated paper (CP) support. Results show that the hydrophilic and electrostatic interactions between the components ensure the integrity of the whole module in aqueous phase dyes, thereby ensuring its practicality and cyclic stability (10 times). Al-fumarate with a superior specific surface area of (1117.82 m 2 /g) and porosity (0.47 cm 3 /g) on the substrate serves to induce and capture the dye molecules, while TiO2 nanoparticles with a wide bandgap trigger a redox reaction to further degrade the organic pollutants . Through the synergistic effect between adsorption and photocatalytic strategies, the resultant functional CP-based composite exhibits superior dye-removal performance than other potential composite materials, reaching 98.93% degradation efficiency of congo red (CR) solution (25 mg/L), and 97.91% elimination capacity of methylene blue (MB) solution (20 mg/L). Therefore, the designed dye-elimination module can serve as a convenient, recyclable, and efficient cleaning module in practical wastewater treatment fields.

CAS / MDL: 7784-13-6
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BIOMATERIALS · 2023 · IF 14

An acid-responsive MOF nanomedicine for augmented anti-tumor immunotherapy via a metal ion interference-mediated pyroptotic pathway

Zhenzhen Feng,Gui Chen,Min Zhong,Ling Lin,Ziyi Mai,Yan Tang,Guimei Chen,Wen Ma,Guang Li,Yuanyuan Yang,Zhiqiang Yu,Meng Yu

Pyroptosis is an inflammatory form of programmed cell death (PCD) that is regulated by the Gasdermin protein family in response to various stimuli, playing a critical role in the development of tumor therapy strategies. However, cancers are generally known to escape from PCD via immunosuppressive pathways or other resistant mechanisms. In this study, an acid-responsive Fe/Mn bimetal-organic framework nanosystem carrying metal ions and immune adjuvant R848 (FeMn@R@H) was designed for combining pyroptosis and augmented immunotherapy. The FeMn@R@H would be triggered to disintegrate and release Fe 3+ and Mn 2+ ions in response to the acidic tumor microenvironment (TME), thereby initiating Fenton-like reactions for ROS-mediated pyroptosis. On the one hand, the pyroptosis-caused cell rupture would induce the release of proinflammatory cytokines and immunogenic constituents from tumor cells, further resulting in immunogenic cell death (ICD) to promote antitumor immune responses. On the other hand, the co-delivered R848 could reverse suppressive tumor immune microenvironment (TIME) and induce inflammatory responses by activating the TLR7/8 pathway. In conclusion, this tumor-specific therapy system can co-deliver metal ions and R848 to tumor tissues to perform pyroptosis-mediated PCD and augmented anti-tumor immunotherapy.

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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

Molecularly imprinted MOF/PAN hybrid nanofibrous membranes for selective bisphenol A adsorption and antibacterial fouling in water treatment

Qiu-hui Hu,De-yu Tang,Xing-han Wang,Ling-ling Yan,Luo-lin Deng,Mei-qi Zhao,Er-ning Deng,Qing-han Zhou

Organic pollutants and microorganisms have become the main challenge in sewage treatment for decades. This mainly results from rapidly developing industry and urbanisation. However, simultaneous clearance of the organic pollutants and microorganisms in water still remains challenging in wastewater treatment. To address this problem, a novel molecularly imprinted metal–organic framework (MOF)/polyacrylonitrile (PAN) hybrid nanofibrous membrane (MOF/PAN-MIM) was prepared for selectively adsorbing bisphenol A (BPA) and inhibiting bacterial fouling in water treatment. Based on the experimental results, the MOF/PAN-MIM showed higher affinity towards BPA as compared to any other organic pollutants and a selective adsorption order of BPA > bisphenol F (BPF) > bisphenol S (BPS) > phenol > nitrophenol > resorcinol with adsorption performance 56.63 mg·g −1 . The kinetics and isotherm models of the adsorption of MOF/PAN-MIM towards BPA are best fitted to a pseudo-second-order mode and a Langmuir isotherm. The cyclic reusability of the membranes was demonstrated by the regeneration experiments, with a removal efficiency of 77.73% towards BPA and a negligible Cu ion leakage of 0.64% after six adsorption–desorption cycles. Additionally, the inhibition rate against E. coli and S. aureus was measured to be greater than 90% via the antibacterial assay. The above results indicated that the as-prepared MOF/PAN hybrid nanofibrous membrane has efficient selectivity, sustained cyclic adsorption ability, and antibacterial fouling effect, which can be used as a potential multi-functional filtration membrane in real wastewater treatment.

CAS / MDL: 75-05-8 9004-64-2
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