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MOLECULES · 2021 ·Vol. 26 ·期 19 ·5736 · IF 4.412

Hydrogenative Ring-Rearrangement of Furfural to Cyclopentanone over Pd/UiO-66-NO2 with Tunable Missing-Linker Defects

Chunhua Wang,Zhiquan Yu,Yuhao Yang,Zhichao Sun,Yao Wang,Chuan Shi,Ying-Ya Liu,Anjie Wang,Karen Leus,Pascal Van Der Voort

Upgrading furfural (FAL) to cyclopentanone (CPO) is of great importance for the synthesis of high-value chemicals and biomass utilization. The hydrogenative ring-rearrangement of FAL is catalyzed by metal-acid bifunctional catalysts. The Lewis acidity is a key factor in promoting the rearrangement of furan rings and achieving a high selectivity to CPO. In this work, highly dispersed Pd nanoparticles were successfully encapsulated into the cavities of a Zr based MOF, UiO-66-NO2, by impregnation using a double-solvent method (DSM) followed by H2reduction. The obtained Pd/UiO-66-NO2catalyst showed a significantly better catalytic performance in the aforementioned reaction than the Pd/UiO-66 catalyst due to the higher Lewis acidity of the support. Moreover, by using a thermal treatment. The Lewis acidity can be further increased through the creating of missing-linker defects. The resulting defective Pd/UiO-66-NO2exhibited the highest CPO selectivity and FAL conversion of 96.6% and 98.9%, respectively. In addition, the catalyst was able to maintain a high activity and stability after four consecutive runs. The current study not only provides an efficient catalytic reaction system for the hydrogenative ring-rearrangement of furfural to cyclopentanone but also emphasizes the importance of defect sites.Keywords:Pd/UiO-66-NO2;furfural;hydrogenative ring-rearrangement;cyclopentanone;double-solvent method

研究领域: 催化化学 · 材料科学
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2024 · IF 4.9

Preparation, formation mechanism, and performance of nitrocellulose aqueous coating based on the anti-solvent method

Xiang Cao,Fengqiang Nan,Wenhao Fan,Heng Gao,Ling Chen,Yan Guo,Weidong He

The organic solvent-based nitrocellulose (NC) coatings exhibit a high volatile solvent content, leading to significant environmental pollution. Whereas, existing waterborne NC-based coating have demonstrated poor water resistance and complex application methods. Therefore, this study aims to develop a green and highly water-resistant waterborne NC-based coating system utilizing a simple anti-solvent method with two environmentally friendly plasticizers , namely acetyl tributyl citrate (ATBC) and triethyl citrate (TEC), as film-forming additives. The dynamic light scattering (DLS) studies revealed that the particle size of NC-based nanoparticles increased with an increase in ATBC content, while it remained relatively constant with an increase in TEC content. Moreover, the particle size results demonstrated that the storage stability of aqueous dispersions containing NC/ATBC (NA) was superior to those containing NC/TEC (NT). Additionally, the physicochemical properties of aqueous dispersions-based films (N dis ), including film formation, hygroscopicity , water resistance, transparency, thermal stability, and mechanical properties were evaluated using solvent-based films (N sol ) as control samples. The results demonstrated that the N dis films exhibited a dense and uniform structure, with physical and chemical properties that were essentially comparable to those of N sol films. However, the mechanical properties of N dis films were somewhat influenced by the nanoparticle size, leading to reduced mechanical performance when the particle size of nanoparticles in the aqueous dispersion was excessively large. The equilibrium moisture content for NA and NT films were reduced to 1.119% and 1.872%, respectively, at a relative humidity of 95%, in comparison to pure NC films (3.975%). Simultaneously, water contact angle measurements indicated an increase from 77° for pure NC film to 89° for NA film and 82° for NT film. All films exhibited superior transparency characteristics. Overall, NA films display excellent water resistance and transparency as well as good mechanical properties.

CAS / MDL: 77-93-0 77-90-7
研究领域: 材料科学 · 环境科学
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Journal of Nanomaterials · 2015 · IF 1.644

Ru Nanoparticles Supported on MIL-101 by Double Solvents Method as High-Performance Catalysts for Catalytic Hydrolysis of Ammonia Borane

Tong Liu,Qingtao Wang,Bingzheng Yan,Mei Zhao,Wenbo Li,Haiyan Bie

Highly dispersed crystalline Ru nanoparticles (NPs) were successfully immobilized inside the pores of MIL-101 by a double solvents method (DSM). HRTEM clearly demonstrated the uniform distribution of the ultrafine Ru NPs throughout the interior cavities of MIL-101. The synthesized Ru@MIL-101 catalyst was also characterized by X-ray diffraction (XRD), N2 adsorption desorption, and ICP-AES. The catalytic test indicated that the Ru NPs supported MIL-101 material exhibited exceedingly high activity and excellent durability for hydrogen generation from the catalytic hydrolysis of amine boranes.

研究领域: 材料科学 · 催化化学
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Nanomaterials · 2024 ·Vol. 14 ·期 11 ·980 · IF 4.4

The Janus Structure of Graphene Oxide and Its Large-Size Conductive Film Strip Pattern

Lu Yi,Xiangnan Chen,Heng Su,Chaocan Zhang

In this paper, the oxidation–exfoliation process of graphite is studied experimentally by the mixed-solvent method, the oxidation–exfoliation process of graphite is simulated theoretically, and it is found that Graphene Oxide (GO) is a Janus structure with inconsistent oxidation on both surfaces; hydrophilic on one side and hydrophobic on the other side. This layer structure and layer spacing are due to the inconsistent oxidation on both sides which changes with the polarity of different solvent mixtures. We used a two-phase system of benzyl alcohol and water, as well as controlling the polarity of the surface of the substrate, to achieve (using a mixed solution of GO which has a selectivity more inclined to the oil phase when the aqueous phase is present) the preparation of reduced graphene oxide patterns. We also used a complex solution of hydrogen iodide and a sodium–iodide complex solution for secondary reduction to enhance its conductivity to 8653 S/m.

研究领域: 材料科学 · 化学工程
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COMBUSTION AND FLAME · 2022 · IF 5.767

Study on nano-boron particles modified by PVDF to enhance the combustion characteristics

Lijuan Yan,Baozhong Zhu,Jiuyu Chen,Yunlan Sun

The existence of an oxide (B 2 O 3 ) film covering the boron (B) surface affects its energy release during combustion. Fluoropolymer modification can help to solve the problem. The electrospinning and solvent anti-solvent methods were utilized to modify boron nanoparticles (n-B) using polyvinylidene fluoride (PVDF) as a modified material, which can effectively coat B particles. The thermal behavior, combustion characteristics, and condensed combustion products of the B/PVDF composites were investigated and evaluated. The agglomeration size of B particles can be decreased while its reaction heat and combustion intensity are increased. Significantly, the combustion performance of the B/PVDF composites prepared by the electrospinning method is better than that of the B/PVDF composite prepared by the solvent anti-solvent method. These results can be helpful in promoting the practical application of B.

CAS / MDL: 68-12-2
研究领域: 材料科学 · 燃烧学
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SURFACE & COATINGS TECHNOLOGY · 2022 · IF 4.865

Study on the preparation and combustion performance of AlF composites prepared by a solvent/non-solvent method

Jingyan Wang,Yaning Li,Zhiwei Han,Saichao Song,Jian Li

Oxidants, such as oxygen, cannot easily approach the core Al due to the presence of dense alumina on the surface of aluminum particles, thereby resulting in high ignition temperature and long ignition duration. To overcome this challenge, we employed the solvent/non-solvent method using Viton A (a copolymer of 1,1-difluoroethylene and hexafluoropropylene) as a coating material to prepare the core-shell Al/Viton A composite particles . An orthogonal experiment was designed to identify the optimal preparation parameters by evaluating the peak pressure in a closed vessel. The sample with the largest peak pressure was compared with raw Al and Al/Viton A (prepared by the physical mixing method) using the combustion pressure and open combustion tests to evaluate the solvent/non-solvent method. The results from the orthogonal experiment revealed that the water bath temperature exhibited the greatest influence on the coating effects. The composite prepared under a water bath temperature of 55 °C and a stirring rate of 250 rpm, using 20 mL of acetone and a 5 mL/min dripping rate of the Viton A acetone solution, were uniformly coated by Viton A, and exhibited excellent combustion characteristics. In addition, the sample generated using the optimal preparation parameters burnt more vigorously and rapidly than raw Al and Al/Viton A. Finally, the reaction molecular dynamics simulation was employed to gain insight into the effect of Viton A on the combustion of Aluminum particles at the molecular level.

研究领域: 材料科学 · 燃烧化学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2025 · IF 6.3

Optimizing alcohol solvents for the synthesis of PtCo alloy catalysts for high-efficient oxygen reduction reaction

Feng Tan,Hao Cui,Dongdong He,Yue Hao,Wenhui Ma,Yunkung Zhao,Yibo Liu,Chengxiong Wang,Feng Liu,Jian Liu,Kezhu Jiang

The polyol solvent thermal reduction method holds great promise for synthesizing Pt-based alloy nanoparticles with commercial viability. However, there is a lack of understanding regarding how various alcohols impact the size, shape, and electrocatalytic properties of particles. To bridge this knowledge gap, we systematically investigated the mechanisms behind the effects of four common alcohols on product characteristics using the polyol solvent thermal method. Our efforts led to the successful synthesis of small, uniformly distributed nanoparticles. Notably, the PtCo/C-BA catalyst, synthesized using benzyl alcohol, exhibited exceptional electrocatalytic activity for the oxygen reduction reaction (ORR). It achieved a remarkable current density of 0.437 A mg −1 and demonstrated minimal mass activity decay after 20,000 cycles. The X-ray Photoelectron Spectroscopy characterization reveals that the PtCo/C-BA catalyst exhibits a higher proportion of metallic-like valence states for Pt and Co, which favors the ORR process. This work not only deepens our understanding of the synthesis strategy but also establishes a foundation for designing high-performance ORR catalysts.

CAS / MDL: 65-85-0
研究领域: 材料科学 · 电化学
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MOLECULES · 2024 ·Vol. 29 ·期 18 ·4452 · IF 4.2

Solvent-Free Method of Polyacrylonitrile-Coated LLZTO Solid-State Electrolytes for Lithium Batteries

Xuehan Wang,Kaiqi Zhang,Huilin Shen,Hao Zhang,Hongyan Yao,Zheng Chen,Zhenhua Jiang

Solid-state electrolytes (SSEs), particularly garnet-type Li6.4La3Zr1.4Ta0.6O12(LLZTO), offer high stability and a wide electrochemical window. However, their grain boundaries limit ionic conductivity, necessitating high-temperature sintering for improved performance. Yet, this process results in brittle electrolytes prone to fracture during manufacturing. To address these difficulties, solvent-free solid-state electrolytes with a polyacrylonitrile (PAN) coating on LLZTO particles are reported in this work. Most notably, the PAN-coated LLZTO (PAN@LLZTO) electrolyte demonstrates self-supporting characteristics, eliminating the need for high-temperature sintering. Importantly, the homogeneous polymeric PAN coating, synthesized via the described method, facilitates efficient Li+transport between LLZTO particles. This electrolyte not only achieves an ionic conductivity of up to 2.11 × 10−3S cm−1but also exhibits excellent interfacial compatibility with lithium. Furthermore, a lithium metal battery incorporating 3% PAN@LLZTO-3%PTFE as the solid-state electrolyte and LiFePO4as the cathode demonstrates a remarkable specific discharge capacity of 169 mAh g−1at 0.1 °C. The strategy of organic polymer-coated LLZTO provides the possibility of a green manufacturing process for preparing room-temperature sinter-free solid-state electrolytes, which shows significant cost-effectiveness.

CAS / MDL: 25014-41-9
研究领域: 材料科学 · 能源技术
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Journal of Materials Chemistry C · 2022 ·Vol. 10 ·期 8 ·3153-3162 · IF 8.067

Self-carbonization synthesis of highly-bright red/near-infrared carbon dots by solvent-free method

Zeyu Zhang,Xiaoyong Chen,Guocheng Fang,Jiajie Wu,Aolong Gao

In biosensing and biophotonics, red/near-infrared fluorescent carbon dots (R-CDs) are attractive and deserve more attention. However, the synthesis and purification of R-CDs are time-consuming, impeding their industrial production and application on a large scale. We proposed a solvent-free method for reducing the number of raw materials used in the R-CD synthesis by utilizing the dehydration self-carbonation effect of the-HSO3 group in the precursor. The synthesized R-CDs exhibit a quantum yield of 59% and an emission wavelength of 600–800 nm with only one raw material (3,4-diaminobenzenesulfonic acid) and without the addition of any extra precursors, solvents, catalysts, dehydration agent, or other additives. We hypothesized that the red/near-infrared emission was caused by carbon-nucleus conjugated structures formed during the dissociation of the –HSO3 group at high temperatures. Additionally, the prepared R-CDs demonstrated a good response to the products of glucose oxidation, indicating glucose's sensing capability. Additionally, the synthesized R-CDs demonstrated excellent single-photon imaging of cells while being non-toxic, demonstrating their enormous potential in biophotonics. We believe that this simple and environmentally friendly R-CD synthesis can significantly accelerate industrialization and application.

研究领域: 材料科学 · 生物传感 · 生物光子学
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CERAMICS INTERNATIONAL · 2022 · IF 5.532

Synthesis of H2TiO3-PVC lithium-ion sieves via an antisolvent method and its adsorption performance

Zhen Yang,Ying Li,Peihua Ma

H 2 TiO 3 is the most promising and highly selective lithium-ion sieve. In this study, HTO-PVC- x ( x  = 10, 15, 20, 25, and 30) lithium-ion sieves were prepared via an antisolvent method using PVC as the matrix. The X-ray diffraction (XRD) and scanning electron microscopy (SEM) results showed that Li 2 TiO 3 was preferentially indexed to a C 2/ c monoclinic structure. LTO-PVC- x had a spherical size of 300 μm and an enormous specific surface area. The morphology and size of HTO-PVC- x obtained by HCl elution were consistent with those of LTO-PVC- x , indicating good separation and recycling properties. HTO-PVC-15 had a higher adsorption performance and adsorption capacity at a lower initial Li + concentration. The adsorption behaviour of HTO-PVC-15 is in accordance with the Langmuir isothermal model and pseudo-second-order model, which belongs to the chemical adsorption process . It reached 96% of its equilibrium adsorption capacity within 2 h. Simultaneously, it maintained high adsorption selectivity and cycling performance and a low Ti 4+ dissolution rate. Thus, HTO-PVC-15 has immense potential to be used for salt lake brine adsorption applications.

研究领域: 材料科学 · 环境工程
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ACS Omega · 2025 · IF 4.3

Particle Size-Controllable Preparation of a CL-20/HMX Cocrystal with High Energy and Low Sensitivity

SongYuChen Ma,Tao Liu,DeQi Wang,YinHui Li,WenJing Shi,FengSheng Li,Jie Liu

To address the quality issues arising from the uncontrollable morphological grain size in the preparation of CL-20/HMX cocrystals, a novel method for producing high-quality cocrystals with well-defined morphological grain sizes has been developed. The cocrystallization process was conducted using the solvent/nonsolvent method, wherein the mixing efficiency and solution supersaturation were precisely controlled through systematic optimization of key parameters, including solvent composition, solvent/nonsolvent ratio, reaction temperature, and stirring rate. Through systematic optimization of experimental parameters, three distinct rhombohedral CL-20/HMX cocrystal samples with uniform particle size distributions and well-defined morphologies were successfully prepared, exhibiting characteristic D50 values of 20, 63, and 130 μm. Comprehensive characterization revealed that SEM analysis demonstrated the cocrystals possess smooth surfaces and regular geometric shapes. Combined XRD and micro-CT analyses confirmed the high crystallinity of the cocrystals, particularly noting the reduced internal defects and superior crystal perfection in larger-grained samples. DSC measurements indicated enhanced thermal stability in cocrystals with larger particle sizes. Furthermore, sensitivity testing showed larger-grained cocrystals are less sensitive than smaller-grained ones, which can be attributed to the more compact internal structure of the crystals.

CAS / MDL: 67-63-0
研究领域: 材料科学 · 爆炸物化学
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Journal of Energetic Materials · 2024 · IF 1.7

Potential reuse of HMX separated from decommissioned propellants: crystallization and characterization of low-sensitivity HMX

Sheng Wang,Sen Hong,Bingxin Liu,Dan Liang,Ling Chen,Yuhua Zhao,Xiao-An Wei

Herein, in order to increase the purity and improve the performance of HMX crude products (Raw HMX) isolated from decommissioned propellants, a new method to obtain submicron levels using the solvent-anti-solvent process was proposed. Two different morphologies of HMX, regular prismatic vs. spherical-like, were obtained by means of two solvents (DMSO, DMF). Polyethylene glycol-200 (PEG-200) was used to improve the morphology and dispersion of crystals at low saturation and low crystallization temperatures. Various rates of addition of anti-solvent (water) were studied to prevent HMX crystalline transition and effectively increase purity. Furthermore, the aging process was applied to further modify the crystals with controlled particle size distribution The purity of the samples was tested by High Performance Liquid Chromatography (HPLC) spectroscopy, and the purity of the crystallized samples was improved from 95.53% in Raw HMX to over 99%. The thermal decomposition properties were investigated by differential scanning calorimetry (DSC) and the kinetic parameters of the thermal decomposition reaction of the materials were calculated using the Kissinger and Ozawa method. The samples were also tested for impact and friction sensitivity, which was reduced compared to both Raw HMX and industrial HMX, demonstrating that this type of modified HMX recovered from decommissioned propellants is fully reusable.

研究领域: 材料科学 · 化学工程 · 爆炸物研究
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