MOLECULES
·
2021
·Vol. 26
·期 19
·5736
·
IF 4.412
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
✓ 已验证
DOI
PubMed
高影响因子
ADVANCED ENGINEERING MATERIALS
·
2020
·Vol. 22
·期 8
·2000162
·
IF 3.217
Qingxiao Meng,Jianyong Feng,Huiting Huang,Xiaopeng Han,Zhi Zhu,Tao Yu,Zhaosheng Li,Zhigang Zou
Both phase and morphology of perovskite films are very important for high-performance optoelectronic devices. Although a two-step method based on CsBr ethylene glycol monomethylether (EGME) solution can prepare pure-phase CsPbBr 3 films, they have a poor morphology due to excessive Ostwald ripening. Herein, a bi-solvent engineering strategy is demonstrated to simultaneously optimize phase and morphology of CsPbBr 3 films in a two-step solution method, which uses the bi-solvents of EGME and isopropanol (IPA) instead of EGME for CsBr solution at the second step. Optimizing the volume ratio of bi-solvents and immersion time can control the Ostwald ripening effectively and result in pure-phase, compact, and smooth CsPbBr 3 films. Finally, the prepared films are applied to perovskite solar cells (PSCs) with a structure of fluorine-doped tin oxide (FTO)/compact TiO 2 (c-TiO 2 )/CsPbBr 3 /carbon. In comparison with EGME, the champion power conversion efficiency (PCE) of devices from EGME/IPA bi-solvents increases from 3.57% to 7.29% owing mainly to higher coverage, smoother surface, and lower trap density of CsPbBr 3 films from EGME/IPA bi-solvents. This work provides a simple and efficient method for the preparation of high-quality CsPbBr 3 films.
研究领域:
材料科学
·
光电子学
✓ 已验证
产品关联
DOI
高影响因子
Nano Energy
·
2022
·
IF 19.069
Chenhui Bai,Xuebiao Li,Xiaojing Cui,Xinru Yang,Xinru Zhang,Kun Yang,Tao Wang,Hulin Zhang
Aqueous thermocells are environment-friendly power sources capable of converting low-grade thermal energy into electricity to power small electronics in various application scenarios free from batteries . However, its poor portability and transparency, mechanical fragility, and low output performance impose a burden on its extensive application. Here, we demonstrate a highly transparent, flexible and stretchable gel with the cross-linked PVA/gelation double network frame by introducing DMSO/water binary solvent to suppress the formation of hydrogen bonds along the three dimensional directions, forming numerous microcrystalline regions. When the temperature difference is 40 K, the gel-based thermogalvanic cell achieves an open-circuit voltage of about 63 mV with the maximum power density of about 1.2 mW m -2 . By implanting a PDMS solar absorber , the assembled solar thermoelectric gel device delivers a maximum temperature difference of about 11.2 K with an open-circuit voltage up to 16.6 mV and short-circuit current of more than 100μA, respectively, upon exposure to sunshine over 12 h. This work may provide new ideas for harnessing ambient heat and solar energy to electrical energy conversion.
研究领域:
材料科学
·
能源技术
✓ 已验证
产品关联
DOI
高影响因子
Journal of Nanomaterials
·
2015
·
IF 1.644
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
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 19
·8930-8939
·
IF 9.931
Yu-Xia Li,Shuai-Shuai Li,Ding-Ming Xue,Xiao-Qin Liu,Meng-Meng Jin,Lin-Bing Sun
Cu(I)-containing materials have great potential in various applications such as in CO adsorption; however, development of an efficient and controllable method to produce Cu(I) sites remains a significant challenge; herein, a two-step double-solvent (DS) strategy is reported for the first time to fabricate Cu(I) sites in a representative metal–organic framework, MIL-101(Cr); this strategy ensures that both introduction of the Cu(II) precursor and its reduction to Cu(I) occur inside the pores and significantly minimizes the aggregation of Cu species. This is difficult to realize through conventional methods used for Cu(II) introduction (wet impregnation) or reduction (liquid-phase reduction). The two-step DS strategy involves selective reduction of Cu(II) to form Cu(I) without the formation of any Cu(0). The obtained Cu(I)-containing materials exhibit an excellent CO adsorption capacity (up to 2.42 mmol g−1) at 298 K and 1 bar, much better than that of the benchmark adsorbents including CuCl/γ-Al2O3 (1.0 mmol g−1), CuCl/MCM-41 (0.57 mmol g−1), and CuZSM-5 (0.11 mmol g−1).
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2023
·Vol. 140
·期 37
·e54417
·
IF 3
Mingjie Lin,Junmei Ma,Xuping Xue,Shiyang Li,Qingyi Wang,Zixuan Lv,Congjie Gao,Linxin Xue
Polyamide (PA) based thin film composite forward osmotic (TFC-FO) membranes were prepared through inter-facial polymerization (IP) processes on porous cellulose acetate (CA) substrates. A dual solvent modification process of adding DMF in the aqueous phase followed by activation with methanol was found to be able to simultaneously improve the permselectivity and anti-fouling capability of the modified membranes. On top of the acidic CA substrates, DMF could not only absorb the HCl formed in the IP processes, but also chemically bind with the PA matrix by reaction with MPD monomers, leading to formation of homogeneous thin and flat PA layers, while methanol activation further swelled the PA matrix, repaired defects and optimized water permeating channels. Using 1 M NaCl solution as the draw solution, the water flux of the CA/PA-DMF4-ME1 membrane was twice that of the pristine membrane, and 24% increase in J w /J s value from 182 to 225 L·mol −1 . Its J w /J s value could be further increased 10 times to 2000 L·mol −1 using 1 M Na 2 SO 4 solution as draw solution. RO tests for the CA/PA-DMF4-ME1 membranes showed 6-fold increase in water permeance, from 1.16 to 7.02 L·m −2 ·h −1 ·bar −1 , as well as increase in NaCl rejection from 94.8% to 97.7% from pristine membrane.
研究领域:
材料科学
·
环境工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2021
·Vol. 168
·期 5
·057526
·
IF 4.316
Mengmeng Xu,Yuhua Dong,Jianbin Zheng
In this article, a core–shell CuPd@UiO-66-NH2 composite material was synthesized by a double-solvent reduction method, and an N2H4 electrochemical sensor based on CuPd@UiO-66-NH2 was constructed. The relationship between the morphology, type, composition, size of the sensor interface composite material and its electrocatalytic performance and sensor response performance was studied, and a new method for detecting N2H4 was established. The surface properties and composition of the materials were studied by transmission electron microscope(TEM),energy dispersive X-ray spectroscopy(EDX) and X-ray diffraction spectroscopy(XRD). The results showed that the synthesized CuPd@UiO-66-NH2 has a regular 3D structure, particle dispersion, and uniform particle size, the particle size is about 90 nm. Electrochemical performance studies showed the sensor is made into detecting N2H4 in a linear range of 0.25 μM ∼ 1.39 mM, with a sensitivity of 386.7 μA·mM−1·cm−2, and a detection limit of 0.08 μM(S/N = 3). Compared with other electrochemical sensors based on metal nanoparticles to detect N2H4, the new sensor exhibited a wider linear range; and its sensitivity was 3 times of that obtained by the Cu-BTC/OMC/GCE. So, the sensor can be used as a potential sensing material to detect hydrazine.
研究领域:
材料科学
·
分析化学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS COMMUNICATIONS
·
2015
·
IF 3.699
Yong Liu,Shao-Yi Jia,Song-Hai Wu,Ping-Li Li,Chun-Jiang Liu,Yi-Ming Xu,Feng-Xiang Qin
Highly dispersed metallic nanoparticles immobilizing inside the pores of MIL-101(Cr) were prepared using double solvent method (DSM). The particle size of Au, Ag, Pd, and AuPd NPs were 2.9 ± 0.7 nm, 1.9 ± 0.6 nm, 2.1 ± 0.6 nm and 2.8 ± 0.7 nm, respectively. The catalytic activity determined by the reduction of p-nitrophenol by NaBH 4 to p-aminophenol of Pd and AuPd prepared by DSM is 9.6 and 8.3 times higher than that of Pd and AuPd prepared by conventional impregnation method. The structure and activity of the catalysts prepared by DSM have no significant changes after three cycles.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
Materials Today Physics
·
2022
·
IF 11.021
Shibo Wang,Fengxian Cao,Weihai Sun,Chunyan Wang,Zhongliang Yan,Nan Wang,Zhang Lan,Jihuai Wu
All-brominated inorganic perovskite CsPbBr 3 has received much attention in the field of optoelectronic applications owing to its superb stability and ease of manufacture under the ambient condition. However, the tedious process and toxic solvent are two major challenges for fabrication of CsPbBr 3 films via a multi-step deposition method . Here, we demonstrate a sustainable bi-solvent system for preparing high-quality CsPbBr 3 films in a triple-step solution-processed route, where the bi-solvent system comprises of green solvent water and ethylene glycol monomethyl ether (EGME) in place of the noxious methanol for CsBr solution. By adjusting the temperature of heat treatment and spin-coating speed, the pinhole-free, ultra-smooth and high crystallinity of CsPbBr 3 films were obtained. As a result, the CsPbBr 3 PSC prepared from the green bi-solvent system demonstrates an optimal power conversion efficiency (PCE) of 9.55%, which is one of the highest efficiencies for planar carbon-based PSCs without hole transport layer. Moreover, the all-inorganic unpacked PSCs exhibit excellent humidity stability under ambient environment for 34 days. Our result not only offers a facile and simple way to fabricate the pure-phase CsPbBr 3 films, but also alleviates the solvent toxicity during the preparation of CsPbBr 3 PSCs.
研究领域:
材料科学
·
光电子学
✓ 已验证
DOI
高影响因子
ACS Applied Nano Materials
·
2021
·
IF 5.097
Run-dong Ding,Dan-dan Li,Yu-lin Li,Jie-hui Yu,Ming-jun Jia,Ji-qing Xu
Ultrafine and well-dispersed PdAu bimetallic nanoparticles (ca. 1.4 nm) are successfully immobilized on amine-containing UiO-66 frameworks (NH2-UiO-66) via a double-solvent impregnation method. By virtue of the double-solvent strategy, the incorporated PdAu nanoparticles (NPs) are mainly present in the alloy state and distributed inside the cavities of NH2-UiO-66 near the window of the cages. The resulting PdAu/UiO-66 catalysts exhibit much higher catalytic activity and stability for the dehydrogenation of formic acid than the catalyst prepared by the conventional single-solvent impregnation method. The composition-optimized Pd0.8Au0.2/UiO-66-D catalyst affords a very high turnover frequency value of 722 h–1 at 298 K, which is among the highest one in the metal–organic framework-supported Pd-based NP catalysts ever reported under similar reaction conditions. The exceptional catalytic activity and stability of Pd0.8Au0.2/UiO-66-D could be mainly attributed to the formation of highly dispersed PdAu alloy NPs, the suitable electronic structure of Pd species adjusted by the alloy effect, and the metal–support interaction, as well as the abundant amine groups that can promote the activation of the formic acid molecule by forming HCOO– under mild conditions.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Jiahui Kou,Lin-Bing Sun
Because of their diverse structure, high porosity, and tunable functionality, metal–organic frameworks (MOFs) are of great interest for diverse applications, including catalysis. However, the poor hydrostability of most reported MOFs hinders their catalytic applications seriously. In addition, the development of an effective method to improve the catalytic activity of MOFs is another challenge. Here, we report for the first time the development of a double-solvent strategy to fabricate MOFs inside silica nanopores. A typical MOF (MOF-5) and a mesoporous silica with two-dimensional hexagonal pore regularity (SBA-15) were first attempted. The double-solvent strategy is based on a hydrophobic solvent and a hydrophilic solution containing MOF precursors with a volume equal to or less than the pore volume of the support so that the MOF can be formed selectively in the channels of support. Our results show that upon confinement in silica nanopores the hydrostability of MOF-5 is apparently improved. The framework of MOF-5 is destroyed obviously in a humid environment for 15 min, but that confined in SBA-15 is well preserved after 8 h. Moreover, the catalytic activity of the composite MOF-5@SBA-15 is superior to that of pure MOF-5 regarding activity and reaction rate. Under the catalysis of MOF-5@SBA-15, the conversion of benzyl bromide in the Friedel–Crafts alkylation reaction can reach 100% at 80 °C for 3 h, which is much higher than that of pure MOF-5 (61%) and SBA-15 (0%). We also demonstrate that the double-solvent strategy can be successfully extended to other MOFs, such as HKUST-1 and ZIF-8. Our work might open up an avenue for the improvement of stability and performance of MOFs, which is highly expected for a variety of applications.
研究领域:
材料科学
·
催化化学
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Pengxiao Liu,Yan Jia,Yao Ning,Xiaocheng Zhang,Shuhui Tian,Fan Yang,Weiyu Song,Ying Zhang
This study demonstrates the significant effect of incorporating inexpensive transition metal nanoparticles into metal-organic frameworks (MOFs) to improve their room-temperature hydrogen storage properties. Low-cost nanoparticles (Cu, Ni, and CuNi) were incorporated into UiO-66(Zr) via the double-solvent approach (DSA) plus chemical reduction processes. All composites exhibited higher hydrogen storage capacity compared to pure UiO-66 at both room temperature and 60 bar. Notably, the hydrogen spillover efficiency of CuNi nanoparticles loaded in UiO-66 was comparable to that of MOF adsorbents embedded with noble metals such as Pd and Pt. The hydrogen storage capacity of CuNi@UiO-66 was significantly increased from 0.20 wt% to 0.74 wt%. DFT calculations showed that the CuNi alloys facilitated the adsorption and dissociation of hydrogen molecules in comparison to the single metal nanoparticles , thus favoring the hydrogen spillover effect and improving the hydrogen storage performance. This work demonstrates the potential of designing MOF loaded with inexpensive metal nanoparticles for optimized room-temperature hydrogen storage.
研究领域:
材料科学
·
纳米技术
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）