RSC Advances
·
2020
·Vol. 10
·期 55
·33444-33449
·
IF 3.119
Jun Liu,Xue Zhao,Haibo Zhang
Today, metal-based nanomaterials play an increasingly important role in the energy, environment, medical and health fields. In order to meet the needs of various fields, it is necessary to continuously develop advanced technologies for preparing metal-based materials. Inspired by previous research, the results of a proof-of-concept experiment show that the hexahydro-closo-hexaborate anion (closo-[B6H7]−) in the borane cluster family has properties similar to NaBH4. Closo-[B6H7]− can not only convert common precious metal ions such as Au3+, Pd2+, Pt4+ and Ag+ to the corresponding zero-valence state, but also convert some non-precious metals such as Cu2+ and Ni2+ to the zero-valent or oxidation state. Closo-[B6H7]− moderate reduction to cause rapid aggregation of metal-based materials is not easy compared with NaBH4. Compared with closo-[B12H12]2−, closo-[B6H7]− achieves the conversion of Pt4+ to Pt0 under ambient conditions, and its reduction performance extends to non-precious metals. The excellent stability and easy modification characteristics determine the universality of the closo-[B6H7]− reduction strategy for metal ions.
研究领域:
材料科学
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化学
·
能源与环境科学
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DOI
PubMed
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
·
2024
·
IF 4
Ya-Nan Yu,Shuai Yang,Xi-Yao Li,Rou Huang,Jie Zhou,Zheng Yin
Ligand with mixed-groups contributes to the construction of special structure motif with novel properties, yet it is challenging to understand and regulate the competitive coordination of different functional groups toward metal ions. Herein, the crystal engineering for MOF construction from two linear di-topic linkers of 4-(1H-tetrazol-5-yl)benzoic acid (H 2 tzba) and the longer 4′-(1H-tetrazol-5-yl)-[1,1′-biphenyl]-4-carboxylic acid (H 2 tzbba) featuring dual groups of phenyl-carboxylate and tetrazole, with three typical 3d metal ions (Mn 2+ , Fe 2+ and Zn 2+ ) were investigated. A series of five new MOFs, that are [Mn 3 (tzba) 3 (dmf) 4 ]·11dmf ( 1 , dmf = N ,N-Dimethylformamide), [Mn(tzba)(H 2 O)] ( 2 ), [Zn 2 (tzba) 2 (dmf)]·0.5dmf ( 3 ), [Fe 2 (tzba) 2 (dmf)]·0.5dmf ( 4 ) and [Zn 2 (tzbbz)(gac)(dmf) 2 ]·1.5dmf ( 5 ), were synthesized under solvothermal reactions. The modified solvent template and temperature effects lead to 3D framework of 1 (dmf solution under 433 K) with [Mn 3 (tz) 3 (COO) 3 ] nodes and 1D hexagonal channels, while the 2 (water solution under 373 K) posssesses compact pillared-layer motif from [Mn 2 (tz) 2 ] nodes. Under changed metal salt reactents but same solvent of dmf, the generated 3 and 4 have isoreticular and porous pillared-layer structure constituted of [M 2 (COO) 2 ] nodes. The use of tzbba coupled with a crucial auxiliary ligand of glycollic acid, leads to 5 as porous pillared-layer MOFs with 1D rounded channels. The porous flexible skeleton of 1 constructed from [Mn 3 ] node with four coordinated dmf facilitates post-synthetic metal exchange of the Mn 2+ by radius similar metal ions following priority of Cu 2+ < Zn 2+ < Ni 2+ < Co 2+ , with maximum exchange percentage ranging from 17 % to 69 %. Time dependent ICP-AES analysis revealed the quite wide feasible solvents for post-synthetic metal exchange, as well as the fine control on substituting degree based on soaking temperature and time. Particularly, the compatible introduce of four different metal ions support the potential of preparing bi-, tri-, tetra- and penta- metal MOF crystals, that can not be obtained by traditional solvothermal reactions.
研究领域:
材料科学
·
化学
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产品关联
DOI
高影响因子
Energy Storage Materials
·
2020
·
IF 16.28
Chuanliang Wei,Huifang Fei,Yuan Tian,Yongling An,Huanhuan Guo,Jinkui Feng,Yitai Qian
Li metal is regarded as the most promising anode for lithium-based batteries due to its extremely high theoretical capacity and the lowest working potential. However, dendrite caused by uneven Li deposition inhibits its practical application. Here we propose a new concept of utilizing amorphous metallic nucleation seeds to induce the uniform deposition of Li. Amorphous 3 °C liquid metal coated on MXene framework is selected as an example for deep investigation. The results indicate that amorphous liquid metal nucleation seeds are stable against MXene and can induce isotropic nucleation and uniform growth of Li. The Coulombic efficiency and performance of symmetric cells are obviously improved both in ether-based and carbonate-based electrolyte under the regulation of amorphous liquid metal seeds. Full lithium metal cells with LiFePO 4 and crumpled MXene nanosheet encapsulated LiMn 2 O 4 cathodes also exhibit better electrochemical performance after modification. Additionally, the concept may be useful for developing other metal based anodes.
研究领域:
材料科学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
Frontiers in Chemical Engineering
·
2021
·
IF 0
Li Guiliang,Liu Yang,Shen Yi,Fang Qile,Liu Fu
Two-dimensional (2D) metal–organic frameworks (MOFs) have emerged as intriguing 2D materials because of their specific features of 2D morphology and designable skeletons, which have elicited great interest in environment remediation. In this work, 2D MOF nanosheets are fabricated via a mixed-solvent solvothermal method, and a regulation strategy of metal inorganic clusters on MOFs is used to construct two different 2D MOFs with monometallic and bimetallic coordination, that is, Ni-MOF and Ni/Cd-MOF. Binary metal coordination renders more crystal defects and vacancies in the framework; thus, compared to monometallic Ni-MOF, bimetallic Ni/Cd-MOF exhibits fewer layers (4∼5 layers), higher specific surface area, larger pore size, and higher surface electronegativity, which leads to its excellent adsorption removal for Pb2+, with higher adsorption rate and affinity, and superior adsorption capacity (950.61 mg/g, almost twice as high as that of monometallic Ni-MOF). Besides, the adsorption mechanism further confirmed that the carboxyl groups (−COO−) from organic linker on 2D MOFs serve as the main binding sites for Pb2+ coordination, and bimetallic Ni/Cd-MOF has more active −COO− sites for Pb2+ capture. Thus, the bimetallic Ni/Cd-MOF regulated by heterogeneous metal atoms shows promising application for highly efficient adsorption of heavy metal ions.
研究领域:
环境科学
·
材料科学
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DOI
Journal of Energy Chemistry
·
2022
·
IF 13.599
Jingjing Cai,Huijun Liu,Yulin Luo,Yuqing Xiong,Lizhu Zhang,Sheng Wang,Kang Xiao,Zhao-Qing Liu
Bimetallic sulfides, integrating the merits of individual components, are ideal structures for efficient electrocatalysis. However, for bimetallic sulfides including metal sulfide heterojunctions (MSH) and single-phase bimetallic sulfides (SBS), it is still unclear about which one has better catalytic activity toward reversible oxygen catalysis and its difference on catalytic mechanism. In this work, we demonstrate a bimetallic sulfide electrocatalyst that could transform from metal sulfide heterojunction (CoS/FeS) to single-phase bimetallic sulfide (CoFeS 2 ) through a facile temperature control strategy. The single-phase bimetallic sulfide (CoFeS 2 ) affords high intrinsic activity, fast reaction kinetics and superior durability toward oxygen evolution reaction (OER) and oxygen reduction reaction (ORR). Density functional theory (DFT) simulations reveal that the (CoFeS 2 ) has homogeneous electron distribution of the CoFeS 2 structure, improves the central energy level of d band, and optimizes the O* and OOH* intermediate and efficiently reduces the energy barrier of the reaction rate-determining step (RDS). The assembled rechargeable zinc-air battery is more stable than the Pt/C and IrO 2 assemblies due to the excellent electrocatalytic activity and stability of CoFeS 2 /NC, suggesting that it has potential for use in practical applications.
研究领域:
材料科学
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电化学
·
理论计算
✓ 已验证
DOI
高影响因子
MOLECULES
·
2019
·Vol. 24
·期 13
·2442
·
IF 3.06
Pengfei Zhuang,Peng Zhang,Kuo Li,Beena Kumari,Dan Li,Xifan Mei
Metal nanomaterials have been reported as effective absorbents for the removal of pollutants in the water system, but the release of ions from these nanomaterials brings another concern. Herein, silver nanoclusters (AgNCs) were encapsulated in porous metal-organic frameworks of ZIF-8 (MOF-AgNCs). Compared to AgNCs, the release of Ag+significantly decreases from MOF-AgNCs, indicating that the product presents a lower threat to the environment. The MOF-AgNCs were employed for the rapid removal of heavy metals, such as Pb2+and Mn2+, from water. The mechanism and removal efficiencies were investigated.Keywords:nanoclusters;metal-organic frameworks;heavy metal ions
研究领域:
环境科学
·
材料科学
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DOI
PubMed
高影响因子
ChemSusChem
·
2013
·Vol. 6
·期 8
·1545-1555
·
IF 7.475
Jinzhu Chen,Shengpei Wang,Jing Huang,Limin Chen,Longlong Ma,Xing Huang
Graphical Acid/Metal Balance : Bifunctional catalysts containing ruthenium and polyoxometalates as active species with a metal-organic framework as support and encapsulation matrix, respectively, are synthesized. Excellent yields in sorbitol are obtained in the conversion of cellobiose and ball-milled cellulose. The evaluation of the balance between the hydrogenation and hydrolysis functions of these bifucntional catalysts reveals that by carefully balancing the ratio of acid site density and the number of metal surface atoms a maximum conversion can be achieved. Cellulose and cellobiose were selectively converted into sorbitol over water-tolerant phosphotungstic acid (PTA)/metal– organic-framework-hybrid-supported ruthenium catalysts, Ru-PTA/MIL-100(Cr), under aqueous hydrogenation conditions. The goal was to investigate the relationship between the acid/metal balance of bifunctional catalysts Ru-PTA/MIL-100(Cr) and their performance in the catalytic conversion of cellulose and cellobiose into sugar alcohols. The control of the amount and strength of acid sites in the supported PTA/MIL-100(Cr) was achieved through the effective control of encapsulated-PTA loading in MIL-100(Cr). This design and preparation method led to an appropriately balanced Ru-PTA/MIL-100(Cr) in terms of Ru dispersion and hydrogenation capacity on the one hand, and acid site density of PTA/MIL-100(Cr) (responsible for acid-catalyzed hydrolysis) on the other hand. The ratio of acid site density to the number of Ru surface atoms ( n A / n Ru ) of Ru-PTA/MIL-100(Cr) was used to monitor the balance between hydrogenation and hydrolysis functions; the optimum balance between the two catalytic functions, that is, 8.84< n A / n Ru <12.90, achieves maximum conversion of cellulose and cellobiose into hexitols. Under the applied reaction conditions, optimal results (63.2 % yield in hexitols with a selectivity for sorbitol of 57.9 % at complete conversion of cellulose, and 97.1 % yield in hexitols with a selectivity for sorbitol of 95.1 % at complete conversion of cellobiose) were obtained using a Ru-PTA/MIL-100(Cr) catalyst with loadings of 3.2 wt % for Ru and 16.7 wt % for PTA. This research thus opens new perspectives for the rational design of acid/metal bifunctional catalysts for biomass conversion.
研究领域:
催化化学
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生物质转化
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材料科学
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产品关联
DOI
PubMed
高影响因子
Science of Advanced Materials
·
2020
·Vol. 12
·期 7
·1078-1089
·
IF 1.117
Xu Hongna,Jin Liguo,Cheng Yan
Metal organic skeleton (MOFs) is a kind of porous material composed of metal ions and organic ligands through coordination, which can be used to absorb a lot of toxic substances from waste water. In this research, UiO-66, UiO-66(Zr) and UiO-66(Zr)–2COOH were synthesized by solvent
thermal method, and physical analysis was conducted on the adsorbent properties of the materials by means of XRD, IR, Zeta potential, etc. In the adsorption test of wastewater impurities, UiO-66(Zr)–2COOH was firstly taken as the research object. With the increase of the initial concentration
of hydrochloric acid, the adsorption capacity of the organic skeleton was greatly increased. However, when the concentration increases further, the growth rate of adsorption decreases, and with the increase of temperature, the adsorption decreases further. The organic skeleton of Hg(II) adsorption
process conforms to the secondary dynamic adsorption model. At the same time, the organic skeleton materials of Hg(II) has strong ability of recognition, the recognition of Hg(II) sex is much stronger than the Ni(II) identification. Uio-66(Zr) and UiO-66(Zr)–2COOH are selected for adsorption
of As, and the adsorption process of the two kinds of materials of As is close to the Freundlich model(III). The ability of absorbing As(III) of these materials is stronger than the ability of As(V). At the same time, UiO-66(Zr)–2COOH shows higher adsorption capacity on the As(III),
and maximum adsorption capacity is 220 mg/g.
研究领域:
材料科学
·
环境科学
✓ 已验证
DOI
高影响因子
Metals
·
2023
·Vol. 13
·期 3
·603
·
IF 2.9
Fanyun Chen,Qingshan Gao,Jing Zhang,Hao Deng,Chen Tian,Zhang Lin
Elemental sulfur is an important non-metallic material that is widely used in various fields including chemical, metallurgical and sulfuric acid industries. Polymetallic sulfur slag (PSS) is an important secondary resource for the recovery of sulfur. However, separation of sulfur from PSS is difficult due to the tight binding of some thiophilic metals to sulfur. Herein, we proposed a recrystallization method for the effective separation of sulfur and metals by using organic solvents to control the particle size of sulfur crystals. It was suggested that the particle size of sulfur recovered in the close to saturation state of toluene is about 2000 μm, while the purity is as high as 99.6%. Moreover, the recovery rate is over 95%, which is more than the current commonly used flotation method. The growth mechanism of sulfur crystals under different saturation conditions lays a foundation for the deepening of the growth theory of large-size sulfur crystals. This method realized the effective separation of sulfur from metal sulfides such as FeS2and ZnS, which provided an important guidance for the recovery of sulfur resources through a novel method of recrystallizing regulation.
研究领域:
冶金学
·
材料科学
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产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2024
·Vol. 31
·期 22
·32935-32949
·
IF 0
Wang Junfeng,Wang Heng,Qi Xianjin,Zhi Gang,Wang Jianhua
The high cost and low adsorption capacity of primary metal-organic frameworks (ZIF-8) limit their application in heavy metal removal. In this paper, Co/Zn bimetallic MOF materials were synthesized with excellent adsorption performance for As 5+ . The adsorption reached equilibrium after 180 min and the maximum adsorption was 250.088 mg/g. In addition, Co-ZIF-8 showed strong selective adsorption of As 5+ . The adsorption process model of Co-ZIF-8 fits well with the pseudo-second-order kinetic model ( R 2 =0.997) and Langmuir isotherm model ( R 2 =0.994), and it is demonstrated that the adsorption behavior of the adsorbent is a single layer of chemical adsorption. In addition, when the adsorbent enters the arsenic-containing solution, the surface of Co-ZIF-8 is hydrolyzed to produce a large number of Co-OH active sites, and As 5+ arrives at the surface of Co-ZIF-8 by electrostatic adsorption and combines with the active sites to generate the arsenic-containing complex As-O-Co. After four cycles, Co-ZIF-8 showed 80% adsorption of As 5+ . This study not only provides a new method to capture As 5+ in water by preparing MOF with partial replacement of the central metal, but also has great significance for the harmless disposal of polluted water.
研究领域:
环境科学
·
材料科学
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产品关联
DOI
PubMed
CHEMOSPHERE
·
2020
·
IF 5.778
Hongyang Wu,Yanfang Huang,Bingbing Liu,Guihong Han,Shengpeng Su,Wenjuan Wang,Shuzhen Yang,Yubin Xue,Shuangqing Li
Hazardous metal pollution became a severe environmental issue in China. An efficient precipitation-flotation process was developed to achieve fast removal for metal-ions from wastewater. Structure and strength of precipitate particles/flocs significantly influence the flotation removal of metal-ions. Formation and growth-evolution of precipitate flocs in precipitate flotation were studied by stage analysis of precipitate particles-formation, flocs-regulation and flotation separation. The results demonstrate that early formed precipitates MHA(humics-metal complexing particles) have small particle size, high fractal dimension, low strength and recovery factor. The addition of Fe 3+ and CTAB(cetyl trimethyl ammonium bromide) reagents make the precipitate particles aggregated to flocs(MHA-Fe, MHA-Fe-CTAB) much more large, loose, coarse, and small-density. The final generated MHA-Fe-CTAB flocs are hard to be broken up, easy to be recovered and efficient to be separated by flotation process. The flotation removal of MHA-Fe-CTAB flocs is clearly higher than that of MHA or MHA-Fe. The flotation results of MHA-Fe-CTAB are as follows: flotation removal of 98.7 ± 0.40%–99.9 ± 0.10%, residual TOC of 0.96 ± 0.38–1.35 ± 0.41 mg/L and turbidity of 0.44 ± 0.09–0.63 ± 0.16 NTU. Introducing Fe 3+ and CTAB reagents into flotation solution contributes to the growth-evolution of precipitate flocs, which could intensify the metal-ions removal via precipitate flotation process and result in more ideal purification indexes for metal-containing wastewater.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Mingjie Li,Zebin Yu,Yanping Hou,Qing Liu,Lun Qian,Cuifang Lian,Xunzheng Rao,Xiaoting Yang
Ga 2 O 3 highlights the high energy band structure for redox reaction. However, information on noble metals and metal oxides deposited Ga 2 O 3 for contaminant elimination and the corresponding mechanisms is still lack. Here, metals and metal oxides deposited Ga 2 O 3 (labeled as M-P and MO-C; M = Ag, Pt, and Pd) were synthesized by photocatalytic and chemical deposition methods and confirmed with XRD and XPS. M-P and MO-C were applied in photocatalytic degradation of three typical contaminants: ciprofloxacin, ronidazole and rhodamine B. The ciprofloxacin and ronidazole degradation rates by Ag 2 O-C and rhodamine B degradation rate by Ag-P were 3.0, 2.7 and 2.4 times as high as those by pure Ga 2 O 3 . This research demonstrates that photocatalytic activities of M-P and MO-C are affected by the types and oxidation states of noble metals, as well as the target contaminants. Potentials of M or MO (E(M Φ ) or E(MO CB ), defined as work function of the metals or conduction band of the metal oxides) is the determining factor for both charge trapping and charge transfer abilities. The highest photocatalytic activity can be obtained when the E(M Φ ) or E(MO CB ) was kept at the level just beyond the single electron reduction potential of O 2 , such as Ag-P and Ag 2 O-C. Finally, the contaminants-specific photocatalytic activities were related to the different functional reactive species. Findings of this study provide important information for the rational design of M and MO deposited photocatalysts.
研究领域:
环境科学
·
材料科学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）