CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Yabing Gan,Guoxing Yin,Zhaomin Xu,Huyang Zhou,Ting Yu,Haitao Li,Peng Yin
Gold (Au) and palladium (Pd) species have been widely used in synthetic chemistry, biology, and environmental sciences, raising hard-to-ignore health and environment risks due to their potential toxicity. Herein, a novel dual-functional fluorescent probe was rationally designed and developed for simultaneous quantification and visualization of Au 3+ and Pd species in the environmental and biological systems. Significant fluorescence enhancement at 484 and 606 nm and color changes were observed upon addition of Au 3+ and Pd 0 with high sensitivity. The detection limit for Au 3+ and Pd 0 was as low as 68 nM and 7 nM, respectively. Combined with smartphone chromaticity and dual-channel fluorescence imaging analysis, this probe was successfully applied to the quantification and visualization of Au 3+ and Pd species in real water samples. Thus, simultaneous naked-eye visualization and quantification of Au 3+ and Pd 0 in real water samples was achieved using this probe. The probe was also successfully applied to fluorescence imaging of Au 3+ and Pd 0 in HeLa cells and zebrafish, promoting the monitor and understanding about gold and palladium species in environmental and biological systems.
研究领域:
环境科学
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生物化学
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分析化学
✓ 已验证
产品关联
DOI
高影响因子
ChemCatChem
·
2025
·
IF 3.9
Jingrong Li,Tingting Xiao,Xinluona Su,Qihang Gong,Peikai Luo,Jian Li,Haiyang Cheng,Fengyu Zhao
Graphical The evolution of the geometric structure and electronic states of Pd species was revealed for Pd/C catalysts in catalyzing the dehydrogenation of 12H-NECZ. The oxidized Pd δ+ species was reduced to Pd 0 species with finely-dispersed on the surface of support to generate H 2 with a high efficiency of 98.3%. The dehydrogenation of liquid organic hydrogen carriers is of significant potential for hydrogen energy applications. We successfully synthesized a highly efficient and stable Pd/C catalyst featuring ultrasmall (2.22 nm) and stable Pd nanoparticles via the deposition–precipitation method for the dehydrogenation of dodecahydro- N -ethylcarbazole. Interestingly, the Pd structure evolves during the reaction, with the Pd 2+ species on Pd/C catalyst re-dispersing into uniformly small-sized Pd 0 nanoparticle under reaction conditions. The conventional thermal treatment of calcination–reduction typically results in larger Pd particles due to the stronger metal-support interaction. Kinetic studies revealed the oxidation state of Pd 2+ species (Pd(OH) 2 , PdO) is more active for the dehydrogenation reaction compared to the metallic state Pd 0 species. The in situ structure evolution induced ultrasmall Pd nanoparticles (2.22 nm) with a constant Pd 0 /Pd 2+ ratio, achieving a high efficiency (98.3%) of H 2 release from 12H-NECZ dehydrogenation at 180 °C. This work provides a simple method for preparing highly dispersed Pd/C catalyst with stable ultrasmall Pd particles, offering valuable insights to researchers in the field of supported metal catalysts.
研究领域:
催化化学
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材料科学
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能源化学
✓ 已验证
DOI
高影响因子
JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
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2022
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IF 4.383
Baogang Su,Qi Zhang,Linjun Shao,Shujing Zhou,Jinjing Li,Yijun Du,Chenze Qi
Heterogeneous palladium catalysts play an important role in the synthetic organic chemistry. Palladium species have been adsorbed on the surface of solid matrices or embedded inside solid matrices to prepare recyclable heterogeneous catalysts. Due to the different surrounding environment, these two type palladium species had different electronic properties and catalytic performances. In this study, we fabricated three series of chitosan composite nanofibers with adsorbed and embedded palladium species. Their fiber morphologies and chemical structures were characterized by SEM and FT-IR, respectively. Positron annihilation lifetime spectra (PALS) showed that the intensities (I 3 ) of o -Ps annihilations were all linearly decreased with the increase of palladium contents in the chitosan composite nanofibers. Moreover, compared with the palladium adsorbed chitosan composite nanofibers, the palladium embedded chitosan composite nanofibers had stronger o -Ps annihilation ability, which could be ascribed to the stronger electron donating property of embedded palladium species and higher crosslinking of chitosan molecules by embedded palladium species. At last, the I 3 values were successfully correlated with the rate constants of chitosan supported palladium composite nanofibers catalyzed Suzuki reactions of iodobenzene with phenylboric acid. Therefore, we have developed a facile method to distinguish the adsorbed and embedded palladium species by PALS, which can be further related with their catalytic performance.
研究领域:
有机化学
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催化材料科学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2017
·Vol. 41
·期 16
·8156-8165
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IF 3.269
Linjun Shao,Chenze Qi
Chitosan microspheres-supported palladium catalysts (Pd@CM) for Mizoroki–Heck reaction have been successfully prepared by electrospraying PdCl2/chitosan mixture in a trifluoroacetic acid (TFA) aqueous solution. Swelling capacity measurement and thermal analysis demonstrated that the palladium species in the chitosan microspheres could cross-link the chitosan efficiently. FT-IR spectra demonstrated that the chitosan in the microspheres could be cross-linked by glutaraldehyde, and the formed Schiff bond could chelate the palladium species efficiently. High resolution transmission electron microscopy (HR-TEM) indicated that the entrapment of palladium species in chitosan microspheres could enhance its dispersion. Mizoroki–Heck reaction catalysis results demonstrated that the catalytic activity of Pd@CM was associated with the size of chitosan microspheres. The Pd@CM with a suitable size was even more active than the catalyst with palladium species adsorbed on the surface of chitosan microspheres (Pd-CM). Moreover, the entrapment of palladium species in chitosan microspheres could reduce its aggregation and leaching in the catalysis procedure, which in turn increased the reusability of Pd@CM catalyst. The high catalytic activity and stability of Pd@CM have been attributed to the entrapment of palladium species within the cross-linked chitosan microspheres and the chelation of palladium species with the abundant amine and hydroxyl groups on chitosan chain.
研究领域:
材料科学
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催化化学
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有机合成
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 15
·7395-7404
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IF 11.301
Qiuyan Duan,Chenghua Zhang,Song Sun,Yang Pan,Xiong Zhou,Yang Liu,Kun Chen,Cunshuo Li,Xianzhou Wang,Wenzhi Li
Lean methane combustion through efficient catalysis is an intensely important way to reduce environmental pollution. Notably, palladium-based catalysts are promising catalytic materials. The small size of palladium particles is a crucial factor to improve the catalytic activity. In this study, we proposed a new pathway to minimize the size of palladium particles for palladium-based catalysts from the perspective of material preparation. We first built double spatial barriers on the interface between the support and the active species to prepare atomically dispersed palladium species catalysts. To be specific, organo-silane was employed as a surfactant to modify the zirconia support and palladium acetate was selected as the palladium precursor, taking advantage of the spatial structure of alkane chains combined with silicon atoms and palladium acetate in toluene. Under a lean methane reaction environment, 0.23 wt% atomically dispersed palladium species deposited on decorated zirconia (donated as 0.23 wt% Pd/SiO2–ZrO2) displayed high catalytic activity with 100% conversion at a temperature of around 400 °C with gas hourly space velocity (GHSV) of 30 000 ml g−1 h−1, higher than that of pristine zirconia loaded with 0.23 wt% palladium nanoparticles (donated as 0.23 wt% Pd/ZrO2), which removed all lean methane at around 600 °C under the same conditions. As the palladium loading increased on the modified support, the 1.38 wt% Pd/SiO2–ZrO2 catalyst had a comparable catalytic activity and fully converted lean methane at around 330 °C. The lean methane combustion reaction pathway for the 0.23 wt% Pd/SiO2–ZrO2 catalyst was investigated by in situ NAP-XPS and in situ DRIFTS. Hydroxyl groups formed during the reaction were transferred to the silica, which could reduce the formation of the inactive Pd(OH)x species and expose more active sites to improve the catalytic activity. It is hoped that this study will provide a novel method to improve the utilization of palladium species in practical applications.
研究领域:
催化化学
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环境科学
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材料科学
✓ 已验证
DOI
高影响因子
RSC Advances
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2017
·Vol. 7
·期 40
·24822-24827
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IF 3.108
Ting Yu,Guoxing Yin,Peng Yin,Ying Zeng,Haitao Li,Youyu Zhang,Shouzhuo Yao
We have synthesized a novel long-wavelength fluorescent probe MFC for detection of palladium (Pd0). This probe not only shows high selectivity for palladium, but also could quickly discriminate different palladium species (Pd0, Pd2+, Pd4+) in phosphate buffered solution. After the reaction with Pd(PPh3)4, the UV absorption of the probe MFC shifts from 334 nm to 594 nm within a few minutes. The probe MFC conjugated with alkyl carbamate, which destroys the principle of intramolecular charge transfer (ICT) and shows weak fluorescence. Based on the Pd0-catalyzed Tsuji–Trost deallylation reaction, the fluorogen was released and the fluorescence intensity at 612 nm was observed with 13-fold enhancement along with an obvious color change from yellow to purple with low detection limit.
研究领域:
分析化学
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材料科学
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催化化学
✓ 已验证
DOI
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2023
·Vol. 37
·期 4
·e7037
·
IF 3.9
Linbo Li,Baogang Su,Linjun Shao,Shujing Zhou,Jinjing Li,Chenze Qi
A series of Schiff-base functional groups modified MCM-41 materials have been synthesized and used as the supports of palladium species. The chemical structures of MCM-41 functionalized by nine Schiff-base functional groups were characterized by Fourier transform infrared spectroscopy (FT-IR), whereas their grafting densities of functional groups were achieved from the results of thermogravimetric analysis (TGA) and elemental analysis (EA). Small angle powdered X-ray (SAX) patterns demonstrate that the ordered mesoporous structures of MCM-41 were well retained after modification of functional groups and immobilization of Pd 2+ cations. Moreover, the regular mesoporous structures of supports and homogeneous dispersions of Pd 2+ cations were characterized by transmission electron microscopy (TEM). The positron annihilation lifetime spectroscopic (PALS) results revealed that the electronic and steric factors of functional groups could affect the o -Ps annihilation properties of support Pd 2+ cations. Meanwhile, the catalytic activities of these supported Pd 2+ cations chelated by different functional groups were determined by the Heck reaction of iodobenzene with n -butyl acrylate. At last, the catalytic activities of these supported Pd 2+ cations were linearly correlated to their o -Ps annihilation properties. This result demonstrates that the catalytic activities of supported Pd 2+ cations chelated by different functional groups can be readily determined by the o -Ps annihilation, which can be potentially used in the design and preparation of highly active palladium catalysts.
研究领域:
化学
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催化科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Guanfeng Tian,Youqing Wu,Shiyong Wu,Sheng Huang,Jinsheng Gao
Synthesizing methanol from CO 2 and green hydrogen is a promising strategy to solve environmental issues and meet the increasing energy demand. In this work, Pd/MnO/In 2 O 3 catalyst with highly dispersed Pd species was prepared via an in-situ reduction method using NaBH 4 as the reducing agent. The highly dispersed Pd species promoted the dissociative of hydrogen and the hydride species could spill over to the MnO/In 2 O 3 due to the strong metal-support interaction between Pd and MnO/In 2 O 3 , which improved the catalytic activity of Pd/MnO/In 2 O 3 for CO 2 hydrogenation to methanol. As a result, the methanol space-time yield of 1 wt% Pd/MnO/In 2 O 3 was 4.8 times higher than that of MnO/In 2 O 3 . Moreover, the methanol selectivity of 1 wt% Pd/MnO/In 2 O 3 was still higher than 70% at a temperature below 280 °C. The present in-situ reduction method is an effective route for the preparation of Pd/MnO/In 2 O 3 catalyst for CO2 hydrogenation to methanol.
研究领域:
催化化学
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环境科学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
MATERIALS CHEMISTRY AND PHYSICS
·
2025
·
IF 4.7
Qingfang Jiang,Wujian Zhang,Weijian Ge,Yiping Jin,Wenfeng Han,Ying Li,Haodong Tang
Sintering deactivation of loaded precious metal catalysts is a pressing issue in the field, significantly reducing catalyst activity. Among them, the redispersion of carbon-loaded precious metal catalysts under a high-temperature atmosphere suffers from the problem of carbon carriers being prone to carbonization. In this study, the sintered PdZn/AC catalysts could be redispersed at low temperatures by adding the additive Zn. Combined with TEM, XRD, XPS, and other characterization means, it was found that the main reason for the redispersion of the sintered catalysts was that the Zn additive could form an alloy with Pd, which promoted the formation of high-valent Pd species, which exfoliated into small particles by oxidation in the O 2 –CO atmosphere. In addition, the factors that influenced the process (Zn content, redispersion temperature, treatment time, and number of treatments) were investigated using the controlled variable method. The present work presents a new idea for recycling sintered precious metal catalysts.
研究领域:
催化化学
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材料科学
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化学工程
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表面化学
✓ 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）