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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2025 · IF 8.3

Thermally converted oxide microstructure on ferritic stainless steel with Cu/Ni dual-layer coating for SOFC interconnect applications

Huixian Weng,Danyang Liu,Shujiang Geng,Gang Chen,Fuhui Wang

Cu/Ni dual-layer coating is applied to improve the performance of SUS 430 steel as solid oxide fuel cells (SOFCs) interconnects. Cu layer is deposited by electroplating, followed by magnetron sputtering Ni layer on top of Cu layer. The coated steels are evaluated in air at 800 °C in correspondence with SOFC cathode environment. Results showed that a considerable amount of Ni diffuses into the steel substrate, while Fe and Cr diffuse from the steel substrate into the coating during the initial oxidation. A (Ni,Fe) 3 O 4 spinel layer is initially formed on the scale surface. Cu diffuses outwards and eventually dopes into (Ni,Fe) 3 O 4 spinel to form (Ni,Fe,Cu) 3 O 4 spinel. The oxide scale evolved into a dual-layer structure of an inner Cr 2 O 3 layer and an outer layer of NiO mixed with spinels after 5 weeks of oxidation. Preoxidation treatment in 800 °C air for electroplated Cu coated steel prior to depositing Ni layer improves oxidation resistance and significantly decreases Cr outward diffusion after 5 weeks of oxidation. Moreover, the oxide scales formed on both Cu/Ni and CuO/Ni coated steels maintain low area specific resistance (ASR) after 5 weeks of oxidation.

CAS / MDL: 7320-34-5
研究领域: 材料科学 · 能源工程
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CERAMICS INTERNATIONAL · 2021 · IF 4.527

Oxidation behavior and electrical properties of metal interconnects with Ce-doped Ni–Mn spinel coatings

Yong Zhang,Yutao Zhang,Caihong Wu,Yiting Yang,Qiang Li,Yongnan Chen

To improve the high-temperature oxidation resistance and electrical conductivity of ferritic stainless steels , protective Ce-doped NiMn 2 O 4 spinel coatings were fabricated on the surface of SUS430 steel by electrophoretic deposition (EPD). The phase structure and microstructure of Ce-doped NiMn 2 O 4 in both powder and coating forms were characterized using X-ray diffraction (XRD) and scanning electron microscopy (SEM). The high-temperature oxidation of the NiMn 2 O 4 spinel coating before and after Ce doping in the air at 800 °C for 168 h was studied by weight gain experiments. The area-specific resistance (ASR) of coatings was measured by a standard four-probe method. It was found that the Ce-doped NiMn 2 O 4 spinel powder displayed a stable structure, high crystallinity, fine grain size, and decreased agglomeration when the Ce content was fixed at 0.05 mol∙L −1 . The oxidation kinetics of NiMn 2 O 4 -coated SUS430 steel before and after Ce doping obeyed a parabolic law with parabolic rate constants of 4.58 × 10 −15  g 2  cm −4  s −1 and 1.83 × 10 −15  g 2  cm −4  s −1 , respectively. When oxidized at 800 °C for 50 h, the ASR value of the coated samples before and after Ce doping stabilized at about 15.2 mΩ∙cm 2 and 14.5 mΩ∙cm 2 , respectively. This work demonstrated that the Ce-doped NiMn 2 O 4 spinel coating improved the high-temperature oxidation resistance and the electrical conductivity of metal interconnects.

研究领域: 材料科学 · 表面工程 · 高温材料
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Nature Communications · 2019 ·Vol. 10 ·期 1 ·1-8 · IF 11.878

Missing-linker metal-organic frameworks for oxygen evolution reaction

Xue Ziqian,Liu Kang,Liu Qinglin,Li Yinle,Li Manrong,Su Cheng-Yong,Ogiwara Naoki,Kobayashi Hirokazu,Kitagawa Hiroshi,Liu Min,Li Guangqin

Metal-organic frameworks (MOFs) have been recognized as compelling platforms for the development of miscellaneous applications because of their structural diversity and functional tunability. Here, we propose that the electrocatalytic properties could be well modified by incorporating missing linkers into the MOF. Theoretical calculations suggest the electronic structure of MOFs can be tuned by introducing missing linkers, which improves oxygen evolution reaction (OER) performance of the MOF. Inspired by these aspects, we introduced various missing linkers into a layered-pillared MOF Co 2 (OH) 2 (C 8 H 4 O 4 ) (termed as CoBDC) to prepare missing-linker MOFs. Transmission electron microscope and synchrotron X-ray measurements confirmed that the missing linkers in the MOF could be introduced and well controlled by our strategy. The self-supported MOF nanoarrays with missing linkers of carboxyferrocene exhibit excellent OER performance with ultralow overpotential of 241 mV at 100 mA cm −2 . This work opens a new prospect to develop efficient MOF-based electrocatalysts by introducing missing linkers.

研究领域: 材料科学 · 电化学
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH · 2024 ·Vol. 31 ·期 11 ·16601-16612 · IF 0

Sunflower-like missing-linker covalent organic framework for efficient extraction of non-steroidal anti-inflammatory drugs

Li Xindi,Deng Xiaojuan,Chen Lei

As excellent crystalline materials, covalent organic frameworks (COFs) are widely used in drug adsorption. In this work, a defective engineering strategy was proposed for designing and preparing the functionalized end-capping monomer and missing-linker COFs. The missing-linker COF 2,4,6-trihydroxybenzene-1,3,5-tricarbaldehyde compound with glycidyltrimethyl ammonium chloride modified benzene-1,4-diamine (TpPa-GTA) was synthesized through Schiff base reaction with wide pore size distribution for adsorption of four nonsteroidal anti-inflammatory drugs (NSAIDs). The adsorption process follows pseudo-second-order kinetics, and the four drugs reached adsorption equilibrium within 10 min. The sunflower-like structure helps to promote intraparticle diffusion during the adsorption process, thereby realizing the rapid adsorption of TpPa-GTA. The equilibrium isotherms fit well with both the Freundlich and Langmuir models, with a maximum adsorption capacity of 83.3–315 mg g −1 calculated from the Langmuir model. Based on the detection results of Zeta potential and XPS, the adsorption mechanism was inferred, and the rapid capture of NSAIDs in the wide pH range of 4.0 to 7.5 was realized under electrostatic interaction, hydrogen bonding, and π-π interaction. The detection of lake and river samples using the missing adapter TpPa-GTA has a recovery rate of 84.2–117%, which provides a new approach to the adsorption of pollutants with COFs.

研究领域: 材料科学 · 环境科学 · 药物化学
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Chemical Science · 2020 ·Vol. 11 ·期 15 ·3978-3985 · IF 9.346

Twist and sliding dynamics between interpenetrated frames in Ti-MOF revealing high proton conductivity

Jing Cao,Wenjie Ma,Kangjie Lyu,Lin Zhuang,Hengjiang Cong,Hexiang Deng

We report the design and synthesis of a titanium catecholate framework, MOF-217, comprised of 2,4,6-tri(3,4-dihydroxyphenyl)-1,3,5-triazine (TDHT) and isolated TiO6 clusters, with 2-fold interpenetrated srs topology. The dynamics of the organic linker, breaking the C3h symmetry, allowed for reversible twist and sliding between interpenetrated frames upon temperature change and the inclusion of small molecules. Introduction of 28 wt% imidazole into the pores of MOF-217, 28% Im-in-MOF-217, resulted in four orders of magnitude increase in proton conductivity, due to the appropriate accommodation of imidazole molecules and their proton transfer facilitated by the H-bond to the MOF structure across the pores. This MOF-based proton conductor can be operated at 100 °C with a proton conductivity of 1.1 × 10−3 S cm−1, standing among the best performing anhydrous MOF proton conductors at elevated temperature. The interframe dynamics represents a unique feature of MOFs that can be accessed in the future design of proton conductors.

CAS / MDL: 10294-33-4
研究领域: 材料科学 · 化学
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Selective lead (II) sorption using aminophosphonate-based sorbents: Effect of amine linker, characterization and sorption performance

Rana R. Neiber,Ahmed A. Galhoum,Ibrahim El-Tantawy El Sayed,Eric Guibal,Jiayu Xin,Xingmei Lu

A one-pot synthesis procedure is designed for preparing two α-aminophosphonate-based-sorbents (DA and TA sorbents). The reaction takes place between amine precursors (two different aliphatic amines with different chain lengths and amino group content; i.e., ethylenediamine (DA) or diethylenetriamine (TA), respectively) and both salicylaldehyde and diphenyl phosphite. Ionic liquid may be used under controlled conditions as an alternative to TiCl 4 catalyst. These materials are first characterized by SEM-EDX, AFM, BET, XRD, FTIR, 1 H-, 13 C-, and 31 P NMR, XPS, TGA, elemental analysis (CHNP), and titration (PZC). Combined with the study of pH effect on Pb(II) sorption, FTIR and XPS analyses are used for exploring the mechanisms involved in metal binding. In a second step, the sorption properties are compared for Pb(II) recovery at pH ≈5. Maximum sorption is influenced by the length of the chain: DA (0.694 mmol Pb g −1 ) > TA (0.494 mmol Pb g −1 ). The sorption isotherms are modelled by the Sips equation for DA (and the Langmuir Dual Site equation) and by the Langmuir equation for TA. Thermodynamic parameters (ΔG°, ΔH° and ΔS°) indicate the spontaneous, endothermic nature and randomness increases during the sorption process. The uptake kinetics (equilibrium reached ≈120 min) is almost equally fitted by the pseudo-first-order rate equation and the pseudo-second-order rate equation. The sorbents show selective Pb(II) sorption against heavy base metals in multi-component solutions. QSAR tools (quantitative activity structure–activity relationships) are used for evaluating the correlation between their intrinsic metal characteristics and their affinities for sorbents. The sorbents are efficiently recycled for at least 5 cycles using 0.2 M HCl as the eluent (loss in sorption and desorption performances ≈10-14% at the fifth cycle, compared with the first cycle).

研究领域: 化学工程 · 环境科学 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Delayed linker addition (DLA) synthesis of dual linker ZIF-8 for separation mono- and di-branched isomers of hexane

Jiayan Zhu,Lin Zhang,Zongjian Liu,Wenxia Zhai,Zhengfei Ma,Qun Cui,Haiyan Wang

The separation of mono- and di-branched C6 alkane isomers is one of the most challenging industrial processes for the production of high-octane gasoline components. In this work, ZIF-8 with dual ligands of imidazole (IM) and 2-methylimidazole (2-MIM), named as DLA-ZIF-8-IM, was synthesized by the method of delayed linker addition, and the microstructure of DLA-ZIF-8-IM was analyzed. Adsorption thermodynamic, kinetic and separation properties of C6 alkane isomers were investigated. The results show that compared with SALE-ZIF-8-IM prepared by the solvent-assisted ligand exchange method, the synthesis method of DLA-ZIF-8-IM is simpler and the BET specific surface area and pore volume (2136 m 2 ·g −1 and 0.72 cm 3 ·g −1 ) of DLA-ZIF-8-IM are increased by 21 % and 14 %, which is more conducive to adsorption and diffusion of 3-methylpentane (3MP) on DLA-ZIF-8-IM. The equilibrium adsorption capacity of 3MP on DLA-ZIF-8-IM reaches up to 2.89 mmol·g −1 , which is 1.1 times than that on SALE-ZIF-8-IM, and the ratio of diffusion time constants between 3MP and 2,3-dimethylbutane (23DMB) on DLA-ZIF-8-IM (5.13) is 2.2 times than that on SALE-ZIF-8-IM. Moreover, at 30℃, the breakthrough adsorption capacity of 3MP on DLA-ZIF-8-IM is 1.46 mmol·g −1 , which is 1.6 times more than that of SALE-ZIF-8-IM (0.90 mmol·g −1 ), while the breakthrough adsorption capacity of 23DMB is basically the same. The separation factor between 3MP and 23DMB on DLA-ZIF-8-IM is 2.96 via the synergy of thermodynamic and kinetic mechanism and the dynamic adsorption capacity of 3MP reaches 1.46 mmol·g −1 . DLA-ZIF-8-IM achieves complete separation of C6 alkane mixtures for obtaining single high-purity product. This work provides a novel synthesis strategy for developing C6 alkane (clear) adsorption separation materials by modulating microporous structures of dual-ligand MOFs.

研究领域: 材料科学 · 化学工程
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JOURNAL OF ALLOYS AND COMPOUNDS · 2022 · IF 6.371

Constructing oxygen vacancies and linker defects in MIL-125 @TiO2 for efficient photocatalytic nitrogen fixation

Libo Wang,Shiyu Wang,Mohan Li,Xue Yang,Fengyan Li,Lin Xu,Yongcun Zou

With the emergence of issues such as global warming and glaciers melting, reducing carbon emissions cannot be ignored. Ammonia can participate in the N element cycle in nature and has a huge market demand. In modern industry, the preparation of ammonia mainly relies on the Haber-Bosch process with huge energy consumption. Using clean photocatalytic method to prepare ammonia can alleviate the above problems. Here, the core-shell structure of MIL-125 @TiO 2 was prepared by post solvothermal method for photocatalytic nitrogen fixation . Linker defects can appear as active sites in the residual MIL-125, which forms an obvious mesoporous structure that accelerates the exchange of electron/mass and promotes the activation of N 2 . The shell structure constructed by thin TiO 2 nanosheets possesses a large specific surface area . And the oxygen vacancies active sites could be highly exposed for nitrogen adsorption and activation, so as to promote the occurrence of the photocatalytic reaction. The O−Ti−N covalent bond is established between the titanium-oxygen clusters in the peripheral of TiO 2 and the linker in MIL-125, which improves the effective separation of electron-hole pairs. The ammonia formation rate of MIL-125 @TiO 2 -2 h is 102.7 µmol g −1 h −1 under simulated sunlight, which is 8 times higher than that of MIL-125. This work provides a novel idea for the preparation of photocatalytic nitrogen fixation materials with controllable structure and multiple active sites.

研究领域: 材料化学 · 光催化 · 纳米材料 · 环境科学 · 能源化学 · 多相催化
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INORGANICA CHIMICA ACTA · 2021 · IF 2.545

Enhanced electrocatalytic hydrogen evolutions of Co(II)phthalocyanine through axially coordinated pyridine-pyrene

Tingting Gu,Isaac Kwaku Attatsi,Weihua Zhu,Minzhi Li,Samuel A. Ndur,Xu Liang

Non-precious metal catalysts can effectively evolve hydrogen in aqueous media, but a highly efficient metal-based catalyst is still a significant assignment. Herein, Co(II)phthalocyanine was noncovalently immobilized on multiwalled carbon nanotubes through axial coordination via pyridine-pyrene linker and applied towards hydrogen evolution reactions. This material provided a superiorly enhanced electrocatalyzed performance signifying high efficiency. With this behaviour, our target material we believe paves the way towards designing efficient energy production and storage devices.

CAS / MDL: 75-09-2 67-63-0
研究领域: 材料科学 · 催化化学 · 能源科学
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MOLECULES · 2024 ·Vol. 29 ·期 14 ·3395 · IF 4.2

Evolution of the Structure and Morphology of Dual-Linker ZIF-301-eIm

Ping Wei,Boyao Xie,Jiang Wang,Yanjun Wu,Qi Shi,Jinxiang Dong

Few studies have reported on the continuous evolution of dual-linker zeolitic imidazolate frameworks’ (ZIFs) structure and morphology during the crystal growth process. Herein, we report the synthesis of a novel ZIF material with CHA topology (ZIF-301-eIm) via the combination of a small-sized 2-ethylimidazole (eIm) with the large-sized 5-chlorobenzimidazole ligand. A series of derivative materials with distinct structures and morphologies were obtained via two pathways: (1) insufficient amount of eIm with prolonged crystallization time (pathway A) and (2) sufficient amount of eIm with prolonged crystallization time (pathway B). Various characterization techniques revealed the continuous evolution of structure and morphology during the crystal growth process. Insufficient amount of eIm and crystallization time (crystallization pathway A) led to ZIF-301-eIm derivatives with defective and open structures alongside an aggregated morphology of nanoparticles. Prolonging the crystallization time allowed small-sized eIm ligands to gradually fill into the framework, resulting in the formation of ZIF-301-eIm-A5 characterized by complete but dense structures with a perfect polyhedral morphology. Remarkably, a sufficient amount of eIm during synthesis (crystallization pathway B) formed ZIF-301-eIm-B1 with a similar structure and morphology to ZIF-301-eIm-A5 in just 1 day. ZIF-301-eIm-B3, with intact, dense structures, exhibits superior acetone/butanol separation performance compared to ZIF-301-eIm-A3 due to small pore windows and large cages facilitating selective adsorption of acetone through exclusion separation.

CAS / MDL: 64-17-5 68-12-2 78-83-1
研究领域: 材料科学 · 化学工程
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ANALYST · 2013 ·Vol. 138 ·期 17 ·4737-4740 · IF 3.969

An enzyme-free and label-free assay for copper(II) ion detection based on self-assembled DNA concatamers and Sybr Green I

Chenchen Ge,Junhua Chen,Wei Wu,Zhiyuan Fang,Lingbo Chen,Qi Liu,Lin Wang,Xuerong Xing,Lingwen Zeng

An enzyme-free and label-free fluorescence turn on biosensor for amplified copper(II) ion (Cu2+) detection has been constructed based on self-assembled DNA concatamers and Sybr Green I. This assay is simple, inexpensive and sensitive, enabling quantitative detection of as low as 12.8 pM Cu2+.

研究领域: 分析化学 · 生物传感器 · 纳米技术
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CHINESE JOURNAL OF CHEMISTRY · 2017 ·Vol. 35 ·期 9 ·1411-1416 · IF 1.852

Ionothermal Synthesis and Structural Characterization of a Novel Open Framework Zinc Diphosphonate with Carboxylate-like Linker

Li Zhang,Lei Liu,Jinxiang Dong

A novel crystalline zinc diphosphonate, (CH 3 NH 3 ) 4 Zn 2 (xbp) 2 •H 2 O, denoted as compound 1 , was ionothermally synthesized from tetraethyl- p -xylylenebisphosphonate (Texbp) and Zn(OAc) 2 in a protic eutectic mixture with urea/methylamine hydrochloride. Its structure was determined by single-crystal X-ray diffraction data and had a special three-dimensional open framework with rhombic channels. Compound 1 belongs to the monoclinic system (space group C2/c ), with lattice parameters a =22.6876(19) Å, b =8.7376(7) Å, c =8.1673(9) Å, β =108.146(2)°, V =1538.5(2) Å 3 , Z =2. Its structure is totally different from the typical organic pillared structure, only two oxygens of the phosphonate group are coordinated with zinc atoms, and the third oxygen exists in the terminal form, which is similar to the popular dicarboxylate linkers in MOFs. The organic cations [CH 3 NH 3 ] + of the eutectic mixture played a structure-directing role for constructing this framework and were confined in the pore channels to balance the negative charges resulting from the zinc phosphonate inorganic chains.

研究领域: 材料科学 · 晶体学
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