GREEN CHEMISTRY
·
2020
·Vol. 23
·期 2
·973-982
·
IF 9.48
Weiwei Wang,Yaqin Zhang,Zifeng Yang,Zhencai Zhang,Wenjuan Fang,Donghui Niu,Hongyan He,Fei Xu
In this study, a series of high-activity imidazole-based dicationic ionic liquids (DILs) were designed and prepared as efficient catalysts for balancing the reactivity between the endo-hydroxyl group (endo-OH) and the exo-hydroxyl group (exo-OH) of isosorbide (ISO) to synthesize high molecular weight poly(isosorbide carbonate) (PIC). Meanwhile, the thermal performance of PIC was precisely optimized by regulating the chain configuration. The results showed that when the trace amounts (4.5 × 10−5 based on the ISO molar amount) of bis-(3-methyl-1-imidazole)-ethylene dibromide ([C2(Min)2][Br]2) were used, the weight average molecular weight (Mw) of PIC reached 98 700 g mol−1. It could be concluded from the results of the experiment and the stimulation that the high catalytic activity of DILs was attributed to the strong electrostatic interaction between the cation and the substrate and the effective balance of the reactivity of the endo-OH and the exo-OH. Furthermore, we found that the reduction of hydroxyl groups in the terminal groups and the increase of endo–endo (a1) structure in the repeating unit improved the thermal properties of PIC. Finally, 1H NMR, Fourier infrared spectroscopy, and density functional theory (DFT) calculations were used to verify the reaction process through anion and cation multi-site synergistic effect and a possible electrophilic–nucleophilic reaction mechanism was successfully obtained.
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高影响因子
Nanoscale
·
2018
·Vol. 11
·期 3
·1058-1064
·
IF 7.233
Yu Ding,Ying Li,Yuanyuan Xue,Boqiang Miao,Shuni Li,Yucheng Jiang,Xien Liu,Yu Chen
Atomically thick ultrathin nanomeshes (NMs) possessing the inherent advantages of both two-dimensional nanomaterials and porous nanomaterials are attracting increasing interest in catalysis and electrocatalysis. Herein, we report a direct chemical synthesis of atomically thick Ni(OH)2-NMs by a NaBH4 assisted cyanogel hydrolysis method, which overcomes the shortcoming of the post-etching method for NM synthesis. Various physical characterization methods show that the as-synthesized Ni(OH)2-NMs have 1.7 nm thickness, a big surface area, abundant nanoholes, and numerous surface/edge atoms with low-coordination numbers. The as-synthesized Ni(OH)2-NMs show a better electrocatalytic performance for the urea oxidation reaction than conventional Ni(OH)2 nanoparticles without holes in the alkaline electrolyte, including a lower onset oxidation potential, faster reaction kinetics, and higher mass activity.
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PubMed
高影响因子
Journal of Cleaner Production
·
2023
·
IF 11.1
Dong Wang,Yumeng Wang,Luheng Jing,Lei Wang,Tonghui Zhang,Xuefen Wang
In this work, a flower-like Fe(OH) 3 @Co 2 (OH) 2 CO 3 catalyst was prepared via the confinement effects provided by L-phenylalanine, which favored the heterostructure construction of active iron centers (Fe(OH) 3 ) anchored on the Co 2 (OH) 2 CO 3 nanosheet supports. Benefiting from the created electron-transfer interface and dual metal active sites, the limitation of redox cycling was broken and exhibited highly efficient catalytic activities , the optimal Fe(OH) 3 @Co 2 (OH) 2 CO 3 catalyst showed comparable catalytic performance for the degradation of dye (degradation degree of 99% methylene blue and orange II within 18 min). In addition, the prepared catalysts were employed for the efficient removal of antibiotics (tetracycline (98.9%), norfloxacin (92.5%) and doxycycline hyclate (90.2%). Besides, the preferred nanofibrous composite membranes prepared by combination of nanofibrous membranes (NFMs) with Fe(OH) 3 @Co 2 (OH) 2 CO 3 catalysts possessed considerable potential for large-scale MB removal (treatment capacity of 238.5 L m −2 and permeability of 191.8 L m −2 h − 1 driven by gravity) and stability (182.7 L m −2 of treatment capacity was achieved in the third run). The strategy of construction of rapid interface-redox on the heterogenous catalysts was designed to enhance catalytic performance, which provided a promising chance for the efficiently large-scale removal of dyes and antibiotics.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2015
·Vol. 26
·期 9
·6612-6624
·
IF 1.569
Wang Jingchao,Wang Linlin,Gao Jun,Zhou Ling,Ge Yunlong,Jing Liqiang,Shi Keying,Li Li
The 3D flower-like mesoporous hierarchical architecture materials were fabricated via a facile one-pot reflux method. The composites were carefully characterized by XRD, SEM, BET, XPS, EIS and MS plot measurements. The results indicated that the morphology of the obtained products could be controlled by adjusting the reaction time, and the sample with the mass ratio of 30 % In(NO 3 ) 2 ·6H 2 O/Ni(NO 3 ) 2 ·6H 2 O (labeled as NIDH-30) formed 3D flower-like mesoporous hierarchical architecture, which was composed of nanopetals with porous thin nanosheets and the size of In(OH) 3 nanoparticles around 8–13 nm. As a result, NIDH-30 exhibited excellent sensing properties at ultra low detection limit of 9.7 ppb for detection of NO x . The response toward 97 ppm NO x could reach to 60 % and the response time was 1.2 s. Moreover, it showed a great selectivity and stability at room temperature. The excellent gas sensing performance could be ascribed to higher surface area and space-charge layer which induce the highly effective surface interaction between the target gas molecules and the surface active sites. Synergetic effect and electronic effect also favoring the effective adsorption of NO x on the surface. All the factors were obviously beneficial for the mesoporous hierarchical Ni(OH) 2 –In(OH) 3 double hydroxide composites as gas sensor for monitoring air pollution.
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JOURNAL OF MATERIALS SCIENCE
·
2020
·Vol. 56
·期 4
·3011-3023
·
IF 3.553
Wang Jing,Li Jing,Liu Yuanyuan,Wang Meiri,Cui Hongtao
The cycling stability of electrode materials is a key for Faraday supercapacitors (FSs), especially the structure-unstable Ni(OH) 2 . There exist various strategies for stabilizing the structure of Ni(OH) 2 such as cobalt ions doping and mechanical support from substrate. However, these strategies have their own disadvantages. On the other hand, the combination of two or more strategies has the serious issues in materials synthesis. In this work, a branched nanosheets-interlaced structure of Co 2+ /Co 3+ -doped Ni(OH) 2 is built by a method of precursor template, which effectively applies two strategies including ions doping and self-supportive structure. Due to the synergistic contribution of these two strategies, the cycling stability of as-prepared material is significantly enhanced. This material also presents excellent high-rate capacity, and the as-assembled asymmetric supercapacitors (ASCs) show both high energy and power densities. These results prove that the effective combination of ions doping and self-supportive structure strategies is a promising route for the preparation of Ni(OH) 2 -based electrode materials with high performance.
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CRYSTENGCOMM
·
2021
·Vol. 23
·期 30
·5200-5207
·
IF 3.545
Qi-Ming Qiu,Guo-Yu Yang
Three new metal borates, namely K0.5[B6O10]·H2O·1.5H3O (1), [GaB5O10]·H2en (2) and NaCs[Ga{B5O9(OH)}{BO(OH)2}] (3), have been synthesized under solvothermal conditions. Compound 1 features an intricate 3D framework composed of [B6O13]8− clusters, resulting in a 6-connected achiral pcu net. After introducing the organic gallium, one of the BO4 groups of the [B6O13]8− cluster is substituted by a GaO4 polyhedron to form the acentric [GaB5O13]8− cluster in 2. It also displays a high second-harmonic generation (SHG) response about approximately 2.6 times that of KH2PO4 (KDP), which is higher than those of alumino-borates (ABOs) containing the acentric [AlB5O13]8− cluster (0.3–2.1 times that of KDP). Dipole moment calculations have been carried out to confirm these results. In the process of trying to synthesize a new compound with a denser structure than 2, we have unexpectedly obtained 3 crystallized in the centrosymmetric (CS) space group, which shows a 1D structure constructed from the [Ga{B5O9(OH)}{BO(OH)2}]2− cluster. This kind of low-dimensional structure is rare in gallo-borates (GBOs) as well as ABOs.
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JOURNAL OF MATERIALS SCIENCE
·
2018
·Vol. 53
·期 24
·16263-16275
·
IF 2.993
Li Jiali,Kong Xianggui,Jiang Meihong,Lei Xiaodong
Up to now, although tremendous effort has been made in exploring Pd-based catalysts for the Suzuki–Miyaura coupling reactions, there is still much room to enhance its catalytic performance by synthesis catalyst with define-designed and tailored structure. Herein, a new kind of Pd-based structured catalyst with hierarchical hollow structure (Pd/Co(OH) 2 /Cu(OH) 2 /copper foam) has been successfully synthesized by three facile steps. As framework, the hierarchical hollow nanoarray structure of Co(OH) 2 /Cu(OH) 2 /copper foam is fabricated by immersion and electrolytic deposition methods. Uniformly dispersed Pd nanoparticles with a narrow size distribution (1.5 ± 0.2 nm) are anchored on the surface of the hierarchical nanotube array through an in situ spontaneous redox reaction between Co(OH) 2 and PdCl 4 2− without any surfactant at room temperature. Compared with other synthesis approaches, it just takes less than 1 h for the whole fabrication process in our strategy, exhibiting very high efficiency. In order to evaluate the catalytic performance of the as-prepared structured catalyst, 16 kinds of reagents were chosen as substrates for Suzuki–Miyaura coupling reaction, exhibiting excellent activity and reusability under mild conditions. We hope this simple and efficient method will open a new strategy to design and prepare structured catalysts.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2024
·
IF 2
Yi Hua,Jinqiu Ma,Shuaiqi Sun,Qingfen Meng,Dan Li,Yong Ma,Lingzong Meng,Guangli Zhou
The water activities and osmotic coefficients in the ternary system NaB(OH)4–Na2B4O5(OH)4–H2O at 323.15 K were investigated with the isopiestic method. The solubilities and physicochemical properties in the NaBO2–Na2B4O7–H2O system at 323.15 K were studied with the isothermal dissolution equilibrium method. The phase diagram in the system consists of two single salt regions for NaBO2·4H2O and Na2B4O7·10H2O, one invariant point saturated with the above salts, and two univariant solubility curves. On the basis of the Pitzer model, the Pitzer binary parameters of Na2B4O5(OH)4 and mixing parameters were fitted with the osmotic coefficients and solubilities. The dissolution equilibrium constant of Na2B4O7·10H2O was calculated with the experimental solubility data and parameters. The calculated solubilities and water activities with the parameters and dissolution equilibrium constants of NaBO2·4H2O and Na2B4O7·10H2O agree with the experimental data.
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INORGANIC CHEMISTRY
·
2016
·
IF 4.82
Hui Yang,Chun-Li Hu,Jiang-Gao Mao
The first examples of mixed-anion lanthanide galloborates, namely, Ln2Ga[B3O6(OH)]2[B7O9(OH)2](CH3CO2)2 [Ln = Y (1), Sm (2), Eu (3), Gd (4), Dy (5)], have been obtained through hydrothermal synthesis. The title compounds are isomorphic and belong to monoclinic space group C2/c (No. 15). Their structures possess [B7O13(OH)2] borate layers further bridged with [B3O7] clusters to give a three-dimensional (3D) borate framework displaying two types of rhombus-like B14O14 14-membered-ring (14-MR) channels along the b axis. The Ga3+ ions are octahedrally coordinated and located at one end of the B14O14 14-MR channels, forming small tunnels of B7Ga 8-MRs, which are filled by the LnIII ions. The Ln ions and Ga cations are further held together by bridging acetate anions. It is worth noting that in these compounds there are two different types of borate clusters and two types of anions that are uncommon in the borates reported. Luminescent studies revealed the characteristic emission bands of Ln ions for compounds 2–5, and the luminescent lifetimes are 3.6, 0.86, and 3.05 ns for compounds 2, 3, and 5, respectively. Magnetic measurements suggest that there are antiferromagnetic interactions between magnetic centers for compounds 2–5.
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INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Guangxin Ren,Baocang Liu,Liang Liu,Minghao Hu,Junpeng Zhu,Xuan Xu,Peng Jing,Jinfang Wu,Jun Zhang
Biomass is a sustainable and renewable resource that can be converted into valuable chemicals, reducing the demand for fossil energy. 5-Hydroxymethylfurfural (HMF), as an important biomass platform molecule, can be converted to high-value-added 2,5-furandicarboxylic acid (FDCA) via a green and renewable electrocatalytic oxidation route under mild reaction conditions, but efficient electrocatalysts are still lacking. Herein, we rationally fabricate a novel self-supported electrocatalyst of core–shell-structured copper hydroxide nanowires@cerium-doped nickel hydroxide nanosheets composite nanowires on a copper mesh (CuH_NWs@Ce:NiH_NSs/Cu) for electrocatalytically oxidizing HMF to FDCA. The integrated configuration of composite nanowires with rich interstitial spaces between them facilitates fast mass/electron transfer, improved conductivity, and complete exposure of active sites. The doping of Ce ions in nickel hydroxide nanosheets (NiH_NSs) and the coupling of copper hydroxide nanowires (CuH_NWs) regulate the electronic structure of the Ni active sites and optimize the adsorption strength of the active sites to the reactant, meanwhile promoting the generation of strong oxidation agents of Ni3+ species, thereby resulting in improved electrocatalytic activity. Consequently, the optimal CuH_NWs@Ce:NiH_NSs/Cu electrocatalyst is able to achieve a HMF conversion of 98.5% with a FDCA yield of 97.9% and a Faradaic efficiency of 98.0% at a low constant potential of 1.45 V versus reversible hydrogen electrode. Meanwhile, no activity attenuation can be found after 15 successive cycling tests. Such electrocatalytic performance suppresses most of the reported Cu-based and Ni-based electrocatalysts. This work highlights the importance of structure and doping engineering strategies for the rational fabrication of high-performance electrocatalysts for biomass upgrading.
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PubMed
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Le Gao,Yawen Li,Guifang Li,Jiaqi Huo,Lishan Jia
Interface engineering as an effective material modification method can regulate local corresponding interfacial geometry and electronic structures, thus enabling a higher intrinsic activity for the oxygen evolution reaction (OER). Herein, we carefully designed p-p heterojunction precursor Co4-MOF@La(HCO 2 ) 3 with internal electric field through electrostatic adherence, which then in-situ transformed into p-p type heterojunction electrocatalyst (Co(OH) 2 )4@La(OH) 3 under KOH activation strategy. The one-step in-situ conversion of (Co(OH) 2 )4@La(OH) 3 generated the interface with significant difference in metal atomic radius and exhibits fascinating nanostructures, which enhances the specific surface area and increases the number of active sites compared with the parent material. Impressively, the obtained material (Co(OH) 2 )4@La(OH) 3 demonstrates satisfying electrocatalytic activity in OER with a low overpotential of only 233 mV to reach a current density of 20 mA cm −2 , and excellent stability for 50 h at 10 mA cm −2 in alkaline medium. In-situ Raman technique indicates that multivalent Co centers are the true active sites during the OER process. Based on density functional theory (DFT) calculation results, La atoms possess empty d orbitals, which are beneficial to facilitate charge transfer from Co to La at the heterojunction interface. Meanwhile, the introduction of La atoms changes the coordinated environment around the adjacent atoms at the interface, which induces the upshift of the d-band center for Co atoms and increases the binding strength of the adsorbed oxygen intermediate.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2020
·
IF 4.65
Weijun Liang,Senlin Wang,Yanxiu Zhang,Jian Gu,Kaida Zhu,Jing Zhong,Xinru Wang
β-Ni(OH) 2 with good crystallinity is grown on the surface of the flower-like α-Ni(OH) 2 to form a 3D α@β-Ni(OH) 2 material by a two-step hydrothermal method . The synthesized β-Ni(OH) 2 is nanometer size and strong alkali stability, while the α-Ni(OH) 2 has a large specific surface, high specific capacity and good electrical conductivity , so there are multiple synergistic effects between the β-Ni(OH) 2 coating and the α-Ni(OH) 2 core. Coupled with a 3D flower-like structure, the obtained α@β-Ni(OH) 2 electrode shows a high capacity of 431 mAh g −1 at a current density of 1 A g −1 . Furthermore, we use the α@β-Ni(OH) 2 electrode and the activated carbon (AC) electrode to assemble an asymmetric supercapacitor (ASC) device. This ASC shows the excellent energy density of 53 Wh kg −1 at a power density of 875 W kg −1 and capacity retention rate of 78% after 5000 cycles. Finally, metal hydride (MH) is used to replace the AC negative electrode, and a cell with a high energy density of 100.17 Wh kg −1 at a power density of 424.75 W kg −1 is obtained. The results show that α@β-Ni(OH) 2 electrode has better electrochemical performance than commercial electrodes and has application prospects in energy storage.
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