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
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
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
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
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）