MOLECULES
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2022
·Vol. 27
·期 17
·5736
·
IF 4.927
Xinxiang Cao,Ruijian Tong,Siye Tang,Ben W. -L. Jang,Arash Mirjalili,Jiayi Li,Xining Guo,Jingyi Zhang,Jiaxue Hu,Xin Meng
Novel zinc–palladium–porphyrin bimetal metal–organic framework (MOF) nanosheets were directly synthesized by coordination chelation between Zn(II) and Pd(II) tetra(4-carboxyphenyl)porphin (TCPP(Pd)) using a solvothermal method. Furthermore, a serial of carbon nanosheets supported Pd–Zn intermetallics (Pd–Zn-ins/CNS) with different Pd: Zn atomic ratios were obtained by one-step carbonization under different temperature using the prepared Zn-TCPP(Pd) MOF nanosheets as precursor. In the carbonization process, Pd–Zn-ins went through the transformation from PdZn (650 °C) to Pd3.9Zn6.1(~950 °C) then to Pd3.9Zn6.1/Pd (1000 °C) with the temperature increasing. The synthesized Pd–Zn-ins/CNS were further employed as catalysts for selective hydrogenation of acetylene. Pd3.9Zn6.1showed the best catalytic performance compared with other Pd–Zn intermetallic forms.Keywords:metal–organic framework;porphyrin;nanosheet;palladium–zinc intermetallic;carbonization;selective hydrogenation;acetylene
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高影响因子
ENERGY
·
2022
·
IF 8.857
Xiaopeng Shi,Pan Li,Xianhua Wang,Jiande Song,Shuqi Fang,Chun Chang,Shusheng Pang
The main purpose of this work was to explore the effect of metal modified biochar and multi-catalysts on improving the quality of products by microwave pyrolysis (MVP) of biomass. Single-component catalysts and multi-catalysts were prepared by Zn/Zr impregnation methods. The prepared catalysts were evaluated by XRD , BET, FT-IR and SEM. The properties, composition and product distribution of bio-oil and bio-syngas were analyzed. The results showed that ZSM-5 obtained more bio-oil (42.16 wt%) at the expense of gas product yield, and BC obtained the highest gas yield (43.10 wt%). Zn promoted the selectivity of aromatic hydrocarbons in bio-oil, Zr could effectively improve the yield of syngas and upgrading bio-oil, respectively. Zr-modified multi-catalyst was prepared, and the highest syngas yield (91.54 vol%) and aromatic hydrocarbon products were obtained. Among them, the selectivity of monocyclic aromatic hydrocarbons (MAHs) reached 21.82%. The mechanism of MVP of biomass under the effect of Zn/Zr modified different catalysts was proposed. The study has successfully demonstrated an approach for producing high-value bio-oil and bio-syngas from microwave multi-catalyst pyrolytic system.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Wenjing Li,Fang Wang,Zhengguo Zhang,Shixiong Min
A self-supported chainmail electrocatalyst is developed by embedding graphitic carbon layer-encapsulated Co nanoparticles on N-doped carbonized wood (Co@NCW) as an advanced air cathode for rechargeable Zn-air batteries (ZABs). The NCW with open aligned microchannels facilitates O 2 and electrolyte permeation and transportation, while the uniformly distributed graphitic carbon layer-encapsulated Co nanoparticles on NCW featuring fast electron transfer kinetics provide abundant triphase reaction sites for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). The Co@NCW exhibits a half-wave potential of 0.89 V vs. reversible hydrogen electrode (RHE) for ORR outperforming the Pt/C (0.85 V vs. RHE) and an overpotential of 410 mV for the OER (10 mA cm −2 ) comparable to RuO 2 (340 mV). A rechargeable ZAB assembled with Co@NCW presents a power density of 47.5 mW cm −2 and excellent stability at 5 mA cm −2 for 240 h. This work provides an effective strategy to fabricate a practically applicable oxygen electrode for ZABs.
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ADVANCED POWDER TECHNOLOGY
·
2022
·
IF 4.969
Ruixue Wu,Xia Zhang,Jinmiao Wang,Lulu Wang,Bin Zhu,Cungang Xu,Guanning Cui,Dongmei Zhang,Yuhua Fan
Two novel Zn-MOFs constructed from 5-hydroxy-2-nitroisophthalic acid (H 2 DIPA) and 5-(4-carboxy-2-nitrophenoxy)-2-nitroisophthalic acid (H 3 BPPA), namely: {[Zn 2 (DIPA) 2 (bimp) 5 ]·DMF·2H 2 O} n ( Zn-MOF 1 ), {[Zn 2 (HBPPA) 2 (bibp) 2 ]·2H 2 O} n ( Zn-MOF 2 ) (bimp = 1,4-di(1H-imidazol-1-yl)butane, bibp = 4,4′-bis(imidazolyl) biphenyl), have been synthesized under solvothermal conditions and characterized by single crystal X-ray diffraction, elemental analysis, IR spectra, powder X-ray diffraction (PXRD) and thermogravimetric analysis (TG). The single-crystal X-ray diffraction analysis indicates that Zn-MOF 1 exhibits an uncommon 3-nodal framework with a (4·6·8)(4·6 3 ·8 2 )(6 6 ) topology, whereas Zn-MOF 1 exhibits an uninodal 4-connected framework with a (4 4 ·6 2 ) topology. Moreover, both of the two Zn-MOFs exhibit exceptional dye adsorption capacities towards the organic dyes with high adsorption rates and excellent adsorption amounts. Particularly, Zn-MOF 1 can selectively adsorb the cationic dye malachite green (MG) whereas Zn-MOF 2 adsorb the anionic dye methyl orange (MO) when there exists another kind of dye in the system. The adsorption process can be illustrated by pseudo-second order kinetic and Langmuir isotherm, and the feasible adsorption mechanism could be the electrostatical interactions, hydrogen bonding between the MOFs and the dyes. Meanwhile, the two Zn-MOFs also show good photocatalytic degradation capabilities toward MB/MV dyes under UV irradiation, and the mechanism studies demonstrate that the main active species are ·OH radicals. Therefore, this functional MOF materials can be treated as a convenient and cost-efficient solution for the sewage handling and environmental protection.
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INORGANIC CHEMISTRY
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2022
·
IF 5.436
Guoxu Qin,Yaqiong Kong,Tianjue Gan,Yonghong Ni
Facile and rapid detection of residual organic pesticides on the fruits and vegetables has recently drawn increased attention in the food safety field. Herein, a surfactant-assisted solvothermal route with subsequent post-modification was designed for the preparation of Eu3+-functionated Zn-BDC ultrathin nanosheets (labeled as Eu3+@Zn-MOF-NS, BDC: 1,4-benzenedicarboxylate) with the thickness of 5 nm. The as-obtained Eu3+@Zn-MOF-NS could be homogeneously dispersed in aqueous systems to form a highly-stable collosol. Under the UV excitation of 325 nm, the as-obtained Eu3+@Zn-MOF-NS displayed red photoluminescence emission of Eu3+ ions, which could be notably quenched by an organochlorine pesticide, 2,6-dichloro-4-nitroaniline (DCNA), without interferences from ions, organic small molecules, and other pesticides. The detection limit and Ksv were 0.17 μM (35 ppb) and 3.2 × 105 M–1 in the water system, respectively. Moreover, the present 2D Eu3+@Zn-MOF sensor was also employed for the detection of DCNA in Chaohu Lake water and tap water and in apple, cabbage, and pakchoi samples with the relative standard deviation (RSD) ranging from 4.74 to 9.77%. Further investigations revealed that the competitive absorption between DCNA and the as-obtained Eu3+@Zn-MOF-NS resulted in the fluorescence quenching of the probe.
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高影响因子
LANGMUIR
·
2022
·
IF 4.331
Xueying Wang,Yang Yang,Rui Wang,Ling Li,Xiaohui Zhao,Wenming Zhang
Herein, we fabricate N-doped porous Ni3S2–Co9S8/carbon aerogels (Ni3S2–Co9S8/NCAs) using carrageenan/NiCo-metal–organic framework (MOF) hydrogels as the precursor via the high-temperature carbonization route with excellent electrocatalytic properties for the oxygen evolution reaction (OER). The electrochemical measurements indicate that the Ni3S2–Co9S8/NCA as a quintessential electrocatalyst exhibits excellent OER performance, which has outperformed most transition metal sulfide (TMS) catalysts in alkaline environments, as attested with a lower overpotential of 337 mV at 10 mA cm–2 and a smaller Tafel slope of 77 mV dec–1. Meanwhile, a Zn–air battery based on Ni3S2–Co9S8/NCA + Pt/C achieves a large power density of up to 256 mW cm–2 (and 193 mW cm–2), small charge/discharge voltage gap, and good cycling stability, notably better than the conventional RuO2 + Pt/C-based Zn–air batteries. These excellent electrocatalytic properties are mainly attributed to the distinct hierarchical porous structure and interfacial synergy between the Ni3S2 and Co9S8 nanoparticle structure with rich defects, facilitating the mass transport and high graphitization degree beneficial for electron mobility. It is envisioned that the research provides a novel approach for the exploration of marine biomass as an electrocatalyst.
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高影响因子
RARE METALS
·
2022
·Vol. 41
·期 8
·2745-2758
·
IF 6.318
Li Pu-Bo,Wang Yong-Xun,Shao Ze-Xi,Wu Bin-Tao,Li Heng,Gao Mang-Mang,Liu Kuan-Guan,Shi Ke-Ren
The Mg–Al layered double hydroxide (LDH) conversion coatings were first synthesized in situ to modify the AZ91D alloy through urea hydrolysis to adjust the pH values (9.4, 10.4, 11.2 and 11.4). The pH 11.2 Mg–Al LDH possessed the best compactness and good crystallinity compared to other in situ LDH coatings and obtained the lowest corrosion current density ( i corr ) of (2.884 × 10 −6 ± 0.345 × 10 −6 ) A·cm −2 , which was attributed to the anion-exchange reaction of LDH and the physical barrier against corrosion owing to the twisted penetration pathway of the interlaced LDH sheets. Core–shell structured Zn–Al LDH@ZIF-8 powder modified with stearic acid (SA) was further wrapped with polyvinylidene fluoride (PVDF) to prepare a hydrophobic double-layered coating on the underlying pH 11.2 Mg–Al LDH (SLLZ). The water contact angle (CA) of the SLLZ coating reached 105.6°, and its i corr decreased to (3.524 × 10 −7 ± 0.214 × 10 −7 ) A·cm −2 compared with a single pH 11.2 film. The SLLZ coating exhibited high durability and corrosion protection, even after 15 days of immersion in NaCl solution. The PVDF, SA and ZIF-8 nano-shells contributed to good hydrophobicity, effectively forming a physical barrier. The Zn–Al LDH core and underlying in situ Mg–Al LDH were beneficial for synergistically promoting anion-exchange reaction between the intercalated anions of LDH and chlorides in corrosive media. This work provides a promising approach that combines core–shell LDH@ZIF-8 with LDH film on a Mg alloy surface to construct a hydrophobic film with excellent long-term anti-corrosion performance. Graphical abstract
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Metals
·
2022
·Vol. 12
·期 1
·149
·
IF 2.695
Chunhui Zheng,Chunlin He,Yingjie Yang,Toyohisa Fujita,Guifang Wang,Wenchao Yang
The continuous expansion of the market demand and scale of commercial amidoxime chelating resins has caused large amounts of resin to be discarded around the world. In this study, the waste amidoxime chelating resin was reutilized as an adsorbent for the removal and recovery of Pb(II), Cu(II), Cd(II) and Zn(II) ions from aqueous solutions. The physical morphology and chemical composition of the waste amidoxime chelating resin (WAC-resin) from the factory was characterized by the elemental analyzer, X-ray photoelectron spectroscopy and Fourier-transform infrared spectroscopy. The influence of the initial metal ions concentration, contact time, temperature and the solution pH on the adsorption performance of the metal ions was explored by batch experiments. It was shown that the optimal pH was 4. Kinetic studies revealed that adsorption process corresponded with the pseudo-second-order kinetic model and the adsorption isotherm was consistent with the Langmuir model. At room temperature, the adsorption capacities of WAC-resin for Pb2+, Cu2+, Zn2+and Cd2+reached 114.6, 93.4, 24.4 and 20.7 mg/g, respectively.Keywords:waste amidoxime chelating resin;characterization;reutilization;heavy metals
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Jia'ni Gong,Pengfei Bai,Yifu Zhang,Qiushi Wang,Jingjing Sun,Yanyan Liu,Hanmei Jiang,Ziyi Feng,Tao Hu,Changgong Meng
Molybdenum trioxide (MoO 3 ) has been widely studied in the energy storage field due to its various phase states and unique structural advantages. Among them, lamellar α -phase MoO 3 ( α -MoO 3 ) and tunnel-like h -phase MoO 3 ( h- MoO 3 ) have attracted much attention. In this study, we demonstrate that vanadate ion (VO 3 - ) can transform α -MoO 3 (a thermodynamically stable phase) to h -MoO 3 (a metastable phase) by altering the connection of [MoO 6 ] octahedra configurations. h -MoO 3 with VO 3 - inserted (referred to as h -MoO 3 -V) as the cathode material for aqueous zinc ion batteries (AZIBs) exhibits excellent Zn 2+ storage performances. The improvement in electrochemical properties is attributed to the open tunneling structure of the h -MoO 3 -V, which offers more active sites for Zn 2+ (de)intercalation and diffusion. As expected, the Zn// h -MoO 3 -V battery delivers specific capacity of 250 mAh·g −1 at 0.1 A·g −1 and rate capability (73% retention from 0.1 to 1 A·g −1 , 80 cycles), well exceeding those of Zn// h -MoO 3 and Zn// α -MoO 3 batteries. This study demonstrates that the tunneling structure of h -MoO 3 can be modulated by VO 3 - to enhance the electrochemical properties for AZIBs. Furthermore, it provides valuable insights for the synthesis, development and future applications of h -MoO 3 .
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高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2023
·
IF 10.9
Zhong-Hui Zheng,Somboon Chaemchuen,Jun-Fei Gu,Jing Hang,Wei Sang,Ji-Chao Wang,Ye Yuan,Cheng Chen
The catalytic alcohol dehydrogenation to carboxylic acids has been demonstrated as an atom-economic and environmental-friendly synthetic method. However, the reported catalysts either require relatively complicated synthesis or exhibit high activity only in the presence of a solvent. Therefore, it is still in high demand to obtain catalysts that feature facile synthesis and perform well even without any solvent. Herein, a series of nanostructured bimetallic Zn/Co species embedded in N-doped hierarchical porous carbon were fabricated in a facile and green manner. More significantly, the best-performing material (Zn/Co@NC-800) was identified as the first heterogeneous catalyst to enable this transformation under solvent-free conditions. Moreover, the as-prepared composites were comprehensively investigated to determine their structural and morphological properties, which rationalized the superiority of Zn/Co@NC-800 over the other synthesized materials. Further studies signified that Co sites (both Co 0 and Co 2+ ) and N species (mainly pyridinic N) were probably involved in this process, functioning as the Lewis acid site and basic site, respectively. Hopefully, this study could provide a simple and sustainable method for carboxylic acid synthesis.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Yeyin Zhang,Ruting Huang,Yong Fang,Jiacheng Wang,Zijie Yuan,Xinwei Chen,Wenjie Zhu,Yuan Cai,Xianyang Shi
This study developed metal–organic frameworks (MOFs) with enhanced properties for CO 2 conversion by doping second- transition metal ions (Ti, Mn, Zn, and Cu) into Fe–MOF, which resulted in Fe-M−MOF (M = Ti, Mn, Zn, or Cu). The selection of different metal species in the metal cluster nodes of the MOFs significantly impacted the CO 2 conversion efficiency. Among the different combinations, the Fe–Cu bimetallic cluster node was identified as the most optimal node. In addition, we investigated various variables and preparation conditions for determining the optimal synthesis conditions for Fe–Cu-MOFs. We observed that a synthesis temperature, time, and pH of 130 °C, 15 h, and 3.2, respectively, yielded the best results. The 13 CO 2 isotope labeling method confirmed that the carbon source of CO and CH 4 were derived from CO 2 . Under simulated visible-light irradiation (λ ≥ 420 nm), Fe–Cu-T130 exhibited the highest photocatalytic activity, with a CH 4 generation rate of up to 444.2 μmol g −1 h −1 . This high activity was attributed to several factors. First, the presence of Fe 2+ , Fe 3+ , and Cu 2+ on the surface of Fe–Cu-T130 resulted in photogenerated electrons and holes under visible-light excitation. Fe 2+ accepted electrons to reduce CO 2 , whereas Fe 3+ and Cu 2+ oxidized H 2 O through holes. Second, the polycrystalline structure of Fe–Cu-T130 with abundant surface oxygen vacancies enhanced the chemical reactivity. Finally, the low conduction band position and narrower bandgap of Fe–Cu-T130 facilitated the excitation of electrons into the conduction band, thereby promoting the CO 2 reduction reaction. This study successfully demonstrated the enhanced photocatalytic activity of Fe–Cu-T130 for CO 2 conversion under visible light. The findings provide insight into the development of MOFs with improved properties for the sustainable and efficient utilization of CO 2 .
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Gengzhe Shen,Jing Kong,Yuqing Fei,Lin Xu,Liuyan Zhang,Xiaohua Jie,De Ning,Zhengjian Chen
In this work, layered double hydroxide (LDH) and reduced graphene oxide (rGO) were incorporated into Zn/Ni matrix coating by cold-spraying on the surface of Mg alloys. Inside the resulting GLG@Zn/Ni coating, LDH/rGO are homogeneously dispersed and inner-connected to a protective network. Compared with other coatings without LDH or rGO nanosheets, the GLG@Zn/Ni coating shows the best corrosion resistance, with a high self-corrosion potential at − 1.174 V (vs. − 1.471 V for Mg), a decent self-corrosion current density of 344.7 μA·cm −2 (vs. 878.3 μA·cm −2 for Mg), and the longest available protection (>720 h) against corrosion. Electrochemical and morphological characterizations reveal a synergistic effect of the coating compositions in enhancing corrosion resistance. In detail, the LDH/rGO network inside the coating restricts the penetration of the corrosive medium, particularly for LDH, which has the capacity to capture corrosive Cl − ions. Meanwhile, Ni promotes the conversion of Zn into passivation layers, which then spread to fill the corrosion pores and interphase cracks. This transformation ultimately leads the GLG@Zn/Ni coating to become a unified whole, providing excellent corrosion resistance.
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