Catalysts
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2023
·Vol. 13
·期 9
·1248
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IF 3.9
Yanni Liu,Yonghui Chen,Yikai Wang,Zijie Xiao,Yilin Chen,Jianchun Jiang,Xiaoping Rao,Yun Zheng
The generation of p-cymene from the catalytic dehydrogenation of dipentene is one of the most vital approaches for the synthesis of p-cymene in the chemical industry. Herein, CTF polymer was synthesized by an ionothermal method via using terephthalonitrile as monomer and NaCl-KCl-ZnCl2ternary mixture as catalyst and solvent, and Pd/CTF catalyst was prepared by loading CTF matrix with Pd nanoparticles via a chemical reduction method. The as-obtained Pd/CTF catalyst with the loading amount of 5 wt% Pd showed remarkable catalytic activity in the dehydrogenation of dipentene to p-cymene with a high conversion rate of 100% and a high selectivity of 96% at the reaction temperature of 220 °C in a stainless-steel autoclave containing 0.1 MPa of Ar gas, and also exhibited good stability in the recycling tests. The strong interaction between Pd nanoparticles and CTF and the enhanced electron transfer at the metal-semiconductor interface contribute to the outstanding catalytic performance of Pd/CTF for the dehydrogenation of dipentene to p-cymene. This work demonstrates that the metal-semiconductor catalysts possessed excellent potential in the production of high-value-added chemical products from terpenes conversion.Keywords:palladium nanoparticles;covalent triazine frameworks;catalysis;dehydrogenation;dipentene
研究领域:
化学工程
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材料科学
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DOI
高影响因子
RSC Advances
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2023
·Vol. 13
·期 35
·24628-24638
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IF 3.9
Ji-qiu Zhang,Yu-Hao Wang,Shu-jing Zhang,Yang-qian Lin,Qing-qing Guan,Xi-meng Xu
Acetylene hydrogenation is a well-accepted solution to reduce by-products in the ethylene production process, while one of the key technical difficulties lies in developing a catalyst that can provide highly dispersed active sites. In this work, a highly crystalline layered covalent organic framework (COF) material (TbBpy) with excellent thermal stability was synthesized and firstly applied as support for ultrasmall Pd nanoparticles to catalyze acetylene hydrogenation. 100% of C2H2 conversion and 88.2% of C2H4 selectivity can be obtained at 120 °C with the space velocity of 70 000 h−1. The reaction mechanism was elucidated by applying a series of characterization techniques and theoretical calculation. The results indicate that the coordination between Pd and N atom in the bipyridine functional groups of COFs successfully increased the dispersibility and stability of Pd particles, and the introduction of COFs not only improved the adsorption of acetylene and H2 onto catalyst surface, but enhanced the electron transfer process, which can be responsible for the high selectivity and activity of catalyst. This work, for the first time, reported the excellent performance of Pd@TbBpy as a catalyst for acetylene hydrogenation and will facilitate the development and application of COFs materials in the area of petrochemicals.
研究领域:
催化化学
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材料科学
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DOI
PubMed
高影响因子
PARTICLE & PARTICLE SYSTEMS CHARACTERIZATION
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2022
·Vol. 39
·期 4
·2200013
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IF 3.467
Xinyi Wei,Jinfeng Zhang,Chang Liu,Xiaopeng Han,Yida Deng,Wenbin Hu
The construction of binary metal Pd-based catalysts is an effective strategy to enhance the activity of methanol oxidation reaction. Herein, atomically dispersed Ir single atoms doped to cuboctahedral Pd nanoparticles (Ir-SAs/Pd) as efficient catalysts for alkaline methanol oxidation are prepared via a simple chemical reduction method. The synthetic Ir-SAs/Pd catalysts exhibit the outstanding mass activity of about 1717.3 mA mg Pd −1 compared with pure Pd and commercial Pd/C in electrooxidation for methanol. Meanwhile, the introduction of Ir single atoms enhances the CO tolerance of Pd nanoparticles to a large extent. On the basis of density functional theory results, the enhanced catalytic performance and CO tolerance rely on the effective improvement of the electron dominance near Fermi level and the negative shift of the d-band center for Pd as a result of the electron redistribution between Pd and Ir atoms. This article will provide new insight into the design of high-performance binary metal catalysts for methanol oxidation in alkaline media.
研究领域:
化学
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材料科学
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催化科学
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DOI
高影响因子
Catalysis Science & Technology
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2012
·Vol. 3
·期 4
·952-961
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IF 0
Maiyong Zhu,Ying Wang,Chengjiao Wang,Wei Li,Guowang Diao
Hollow carbon nanonets (HCN), which are attractive materials for catalyst support, were fabricated using the pre-synthesized hematite nanoparticles as the hard template. And then the HCN supported Pd nanoparticles (Pd/HCN) were prepared by precipitation-reduction method. The catalytic performance of Pd/HCN was investigated using Suzuki and Heck coupling reactions as model reactions. The results demonstrated that the as-prepared Pd/HCN nanocomposites exhibit high catalytic activity for the two types of coupling reactions under ligand free conditions. Especially, the Suzuki reactions between various aryl halides and phenylboronic acid gave excellent yields in water. Moreover, the as-prepared Pd/HCN catalysts can be easily recovered from the reaction medium by centrifugation for recycling, and the catalytic efficiency shows no obvious loss even after 6 repeated cycles.
研究领域:
材料科学
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化学工程
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纳米技术
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DOI
Catalysis Science & Technology
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2012
·Vol. 2
·期 11
·2332-2340
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IF 0
Jiefeng Hu,Yuping Wang,Min Han,Yaoming Zhou,Xiaoqing Jiang,Peipei Sun
Fe3O4 and Pd nanoparticles were assembled on sulfonated graphene (s-G) by an easy chemical approach and characterized by transmission electron microscopy, X-ray diffraction and energy dispersive X-ray spectroscopy. The resulting material could be dispersed homogeneously in water or water/ethanol and further used as an excellent semi-heterogeneous catalyst for the Suzuki–Miyaura cross-coupling reaction in an environmentally friendly solvent under ligand-free ambient conditions. The high heterogeneous catalytic activity appears to be due to the small size of Pd nanoparticles and homogeneous distribution of the nanoparticles on the Fe3O4/s-G matrix. In addition, the catalytic activity did not deteriorate even after repeated applications, which may be due to the easy and efficient magnetic separation of the catalyst and the high dispersion and stability of the catalyst in an aqueous solution.
研究领域:
材料科学
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催化化学
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DOI
Catalysis Science & Technology
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2014
·Vol. 5
·期 1
·572-577
·
IF 4.76
Fengwei Zhang,Hengquan Yang
A simple, efficient and recoverable palladium-based catalyst was successfully prepared by immobilizing palladium nanoparticles (Pd NPs) over hydrophobic core–hydrophilic shell structured mesoporous silica microspheres. The obtained catalyst was characterized by transmission electron microscopy (TEM), N2 adsorption–desorption, Fourier-transform infrared spectroscopy (FTIR), thermogravimetric analysis (TGA) and X-ray photoelectron spectroscopy (XPS). The as-prepared catalyst could rapidly convert phenol to cyclohexanone with 98.5% conversion and 97.1% selectivity under mild reaction conditions in the aqueous phase (1 atm H2, 80 °C, 3 h). The excellent catalytic performance of the Pd/MS-C3@MS-NH2 catalyst was probably attributed to the enhanced synergistic effect between highly dispersed Pd NPs and significantly decreased phenol mass transfer resistance. In addition, it could be easily recovered by centrifugation and reused 5 times without any significant loss in activity and selectivity.
研究领域:
材料科学
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催化化学
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环境化学
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DOI
高影响因子
Journal of Energy Chemistry
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2024
·
IF 14
Shaobo Zhang,Yabo Guo,Lu-Hua Zhang,Zhihao Feng,Bo Zhang,Yaheng Wang,Fengshou Yu
Electrochemical nitrite reduction reaction (NO 2 − RR) is a potential sustainable route for regulating the nitrogen cycle and ambient ammonia (NH 3 ) synthesis. However, it remains a challenge to precisely regulate the reaction pathways and inhibit competing reactions (e.g. hydrogenolysis) for efficient and selective NH 3 production in an aqueous solution environment. Here, we utilize the Schottky barrier-induced surface electric field to construct high-density electron-deficient Pd nanoparticles by modulating the N content in the carbon carrier to promote the enrichment and immobilization of NO 2 − on the electrode surface, which ensures the ultimate selectivity for NH 3 . With these properties, Pd@N 0.14 C with the highest N content achieved excellent catalytic performance for the reduction of NO 2 − to NH 3 with the 100% Faraday efficiency at −0.5 and −0.6 V vs. reversible hydrogen electrode (RHE) for NH 3 production, which was significantly better than Pd/C and Pd@N x C samples with lower N content. This study opens new avenues for rational construction of efficient electrocatalysts for nitrite removal and NH 3 electrosynthesis.
研究领域:
环境科学
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电化学
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材料科学
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
·
IF 3.9
Bin Zhang,Xiaodong Guo,Xin Feng,Xiaoxia Duan,Guilong Wang,Chao Yang
The debenzylation reaction of hexabenzylhexaazaisowurtzitane (HBIW) and 2,6,8,12-tetraacetyl-4,10-dibenzyl-2,4,6,8,10,12-hexaazaisowurtzitane (TADBIW) to synthesize 2,6,8,12-tetraacetyl-2,4,6,8,10,12-hexaazaisowurtzitane (TAIW) is the major challenge in the production of 2,4,6,8,10,12-hexanitro-2,4,6,8,10,12-hexaazaisowurtzitane (HNIW). This is primarily attributed to the reaction needing a lot of palladium catalysts, which tend to deactivate rapidly during the process. In this work, a series of Pd(OH)2/C catalysts were successfully prepared through a convenient deposition-precipitation method by controlling the flow rate of the PdCl2 solution. Employing the 10% Pd(OH)2/C–F0.5 sample, the debenzylation reaction was successfully completed with a lower usage of Pd and shorter time of reaction. For the HBIW debenzylation reaction, the yield of TADBIW was 87.4% at low temperature (25 °C) when 1‰ Pd/HBIW was used, and the higher yield was 89.8% at high temperature (45 °C) when 3‰ Pd/HBIW was used. The TADBIW/Pd/h values of them were 42.5 and 95.7, respectively. For the TADBIW debenzylation reaction, the complete conversion of the reactant was realized when Pd/TADBIW was 2‰. The value of TAIW/Pd/h was 154.6 when Pd/TADBIW was 4‰, which was higher than the reports. Compared to the reported catalysts, the dosage of Pd used in the debenzylation reactions of HBIW and TADBIW was significantly decreased. Furthermore, the 10% Pd(OH)2/C–F0.5 sample was recycled six times with similar performance, demonstrating excellent stability. Based on the analysis of characterization results, it is effortless to find that the flow rate of the PdCl2 solution plays a key role in controlling the adsorption behavior of palladium species on activated carbon. The lower flow rate is beneficial to obtaining Pd nanoparticles with a smaller size, a higher proportion of Pd2+, and a higher metal distribution. This study may provide a simple way to develop palladium catalysts with high performance for related applications.
研究领域:
化学工程
·
催化材料科学
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DOI
高影响因子
JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
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2024
·
IF 4.3
Xudong Huang,Haifeng Chen,Zhengjun Shi,Guiying Xing,Linjun Shao,Chenze Qi
Supported palladium catalysts have garnered much interest in the modern chemical industry due to their high catalytic activity and excellent recyclability. Carbon nanofibers are outstanding supports for palladium species because of their large surface areas and chemically inert properties. Herein, with poly(vinylpyrrolidone) as the co-spinning agent, palladium cation embedded polyimide nanofibers were first prepared by electrospinning and thermal imidization. Then, these composite nanofibers were carbonized to prepare palladium embedded nitrogen doped carbon nanofibers. It was found that raising the carbonization temperature could reduce the fiber diameter and increase the size of micropores in the fiber. Meanwhile, the Pd 2+ cations in the nanofibers were reduced to Pd 0 nanoparticles and their sizes grew with the increase of carbonization temperature. The palladium nanoparticles were partially or totally embedded inside the carbon nanofibers. Suzuki reaction catalysis results show that these palladium embedded carbon nanofibers could effectively catalyze the Suzuki reactions of aromatic iodides and bromides with phenylboronic acid to afford the biaryl products with excellent yields. Moreover, this fibrous catalyst can be readily recovered by filtration and reused for 5 times with little loss of initial activity. The remarkable catalytic efficiency and stability of this novel palladium embedded carbon nanofibers could be attributed to the embedment of palladium nanoparticles and chelation of doped nitrogen atoms in the carbon fibers.
研究领域:
材料科学
·
催化化学
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产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
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2024
·
IF 4
Zhiru Li,Ying Lv,Xuelian Chen,Meixia Xiao,Lei Wang,Xiaoxuan Li,Yumin Li
Aiming at the challenges such as wide band gap, limited surface reactivity, and sluggish reaction kinetics of the promising Aurivillius compound Bi 2 O 2 (OH)NO 3 (BON). Our endeavors culminated in the successful creation of layered BON nanoplates featuring surface oxygen vacancies and Pd nanoparticles deposition by UV light irradiation, elegantly designated as Pd-OVs BON. This accomplishment was realized through the adept application of a two-step photoreduction technique, skillfully executed in both pristine water and ethanol-water environments. We then evaluated the effectiveness of Pd-OVs BON in degrading a series of tetracycline antibiotics. Our evaluation involved a comprehensive approach, encompassing systematic morphology characterization and photoelectrochemical analysis. Additionally, we investigated how surface oxygen vacancies and the plasma effects of Pd impact the separation and transport of photogenerated carriers, as well as the photocatalytic performance. The outcomes of this study indicate that Pd-OVs BON holds substantial potential for the photodegradation of antibiotics. Its layered nanoplates structure enhances the specific active surface area of BON, while the surface oxygen vacancies generated through photoreduction create more active sites for catalyzing antibiotic degradation reactions. Furthermore, the introduction of Pd nanoparticles onto the OVs-BON surface during the secondary photoreduction process induces localized surface plasmon resonance. This phenomenon broadens the photocatalyst's responsiveness to a wider range of light wavelengths, enabling efficient utilization of visible light and facilitating the effective decomposition of antibiotic molecules.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
Laser & Photonics Reviews
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2024
·
IF 9.8
Changrui Liao,Haoqiang Huang,Mengqiang Zou,Ying Wang,Shangben Jiang,Dezhi Zhu,Jiabin Huang,Jiajun Guan,Famei Wang,Cong Zhao,Mengjie Zheng,Weijia Bao,Dejun Liu,Xiaoyu Weng,Liwei Liu,Junle Qu,Yiping Wang
Optical fiber hydrogen (H 2 ) sensors have garnered attention for avoiding explosion hazards in flammable gas environments. Conventional optical fiber sensors rely on electron beam sputtering and chemical coating for functionalization, but these methods may not achieve precise functionalization of intricate structures. Based on 4D printing principles, an H 2 -sensitive ink containing methacrylate groups modified palladium (Pd) nanoparticles (NPs) is reported, with a printing resolution of 200 nm. Then, a fiber-tip clamped-beam H 2 sensor is fabricated with the femtosecond (Fs) laser-induced two-photon polymerization (TPP) technique. The sensor exhibits compact dimensions and fast responses, only 2.64 s for a 4.0 vol.% H 2 concentration. A high sensitivity of roughly 165 pm % −1 is achieved as the H 2 concentration increases from 0% to 5.5 vol.%. This study demonstrates that H 2 -sensitive microstructures can be flexibly achieved by TPP of H 2 -sensitive inks, offering a solution for achieving on-chip direct laser writing of integrated H 2 microsensors.
研究领域:
材料科学
·
光学工程
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
International Journal of Electrochemical Science
·
2023
·
IF 1.5
Jing Leng,Ping Li,Ling Bai,Yingqiong Peng,Yongfang Yu,Limin Lu
A Pd nanoparticles-graphene oxide (PdNPs/GO) hybrid as a highly sensitive sensing platform for determination of rutin was successfully prepared by a facile one-pot redox synthesis approach. Formation of PdNPs and loading onto the GO nanosheets were accomplished simultaneously by a redox reaction between H2PdCl4 and GO, without use of any additional reductants. Scanning electron microscopy (SEM) results demonstrated that PdNPs with an average size of 60 nm were distributed on the surface of GO nanosheets. Compared with the GO modified electrode, the PdNPs/GO modified electrode showed a better electrocatalytic activity toward the oxidation of rutin with larger peak current. Then the PdNPs/GO hybrid can be used as an enhanced sensing platform for the electrochemical determination of rutin. Under the optimal conditions, the anodic peak current was linear to the concentration of rutin in the range from 0.005 to 6 μM with the detection limit of 0.001 μM (S/N = 3). More importantly, the developed sensor can be used for the determination of rutin in medicine tablets with satisfactory results.
研究领域:
材料科学
·
分析化学
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药物分析
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DOI
高影响因子
危险品化学品经营许可证（带存储）