JOURNAL OF MATERIALS SCIENCE
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2024
·Vol. 59
·期 45
·21027-21039
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IF 3.5
Zhang Peng,Guo Mengya,Wang Fujiang,Tang Qiong,Ge Hui,Guo Shuke,Zhou Ligong,Li Xuekuan,Dong Jinxiang,Tang Mingxing,Liu Lei
Selective hydrogenation is an effective approach to utilize coal tar and slurry oil to produce high value-added fine chemicals. However, how to efficiently improve the selectivity of the target product and the stability of the catalyst is difficult. Herein, the PdZn alloy catalyst was synthesized by the assistance of strong interaction between active metal (Pd) and support (ZnO) for hydrogenation of anthracene to symmetrical octahydro anthracene (sym-OHA). The PdZn alloy catalyst reduced at 400 °C was found to exhibit a 100% conversion of the anthracen with 84.77% selectivity to sym-OHA under the optimized conditions (200 °C, 1 MPa). The characterization analysis indicated that the PdZn alloy with electron-rich Pd active sites is more efficient in the selective hydrogenation than the pure Pd metal. The study of the deep hydrogenation of sym-OHA (Hydrogenation of sym-OHA to perhydroanhtracene) showed that PdZn alloy catalysts were inactive to further hydrogenation of sym-OHA. Additionally, due to the strong interaction between Pd and ZnO, the Pd/ZnO(400) catalyst shows high stability for five cycles. These findings are of practical significance for the selective hydrogenation of polycyclic aromatic hydrocarbons (PAHs) to produce high value-added products.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2019
·
IF 4.084
Zilong Zeng,Guoliang Liu,Jiafeng Geng,Dengwei Jing,Xinlin Hong,Liejin Guo
Methanol steam reforming (MSR) is deemed to be an effective way for hydrogen production and Pd/ZnO catalyst were found to exhibit high activity in this reaction. However, their activities are strongly related to the preparations methods. In most cases, these catalysts are synthesized by impregnation or co-precipitation methods, aiming to change the dispersion and stability of Pd nanoparticle to get better performance. Here we report an efficient Pd/ZnO catalyst that was synthesized with zeolitic imidazolate framework-8 (ZIF-8) as the precursor, on which Pd ions was supported after NaHB 4 reduction. Typically, when the catalyst reduced at 300 °C for 2 h, the methanol conversion could reach 97–98% and the CO 2 selectivity is around 86.3% under the reaction condition of 0.1 MPa, water/CH 3 OH = 1.2:1 (mol ratio), WHSV methanol = 43152ml/g cat *h, catalyst = 0.1 g, our catalyst was found to show much better performance than other Pd@ZnO catalysts prepared by other methods, especially in terms of selectivity which is particularly important for hydrogen fuel cell application considering that Pt electrode could be poisoned by even trace amount of CO. It turned out that the large surface area , enough holes, evenly distributed PdZn alloy activity sites and abundant oxygen vacancies lead to the overall excellent performance of our catalyst.
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 ALLOYS AND COMPOUNDS
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2023
·
IF 6.2
Mingzhi Chen,Sifan Zhang,Chenyu Zhu,Huan Zhang,Lihua Zhu,Yingliang Feng,Jiexiang Wang,Qian Yang,Bingqian Liu,Wentao Xu
MOFs (metal-organic frameworks) materials have been widely applied in sensing and catalysis, with the advantages of large surface area, numerous active sites, controllable size and morphology. Herein, we report the preparation of the caged PdZn/NC catalysts with the PdZn alloy nanoparticles on carbon doping with nitrogen owing high electrocatalytic performance by using a hydrothermal synthesis and pyrolysis strategy. The caged structure and PdZn alloy are demonstrated by a series of advanced characterization techniques. The material combines the advantages of bimetallic alloy and MOFs cage structure to realize highly efficient electrocatalytic oxidation of ethanol oxidation reactions (EOR) and methanol oxidation reactions (MOR) simultaneously. Electrochemical test results show that PdZn/NC-2 has a mass activity of 2.41 A mg −1 pd and 2.64 A mg −1 pd for methanol and ethanol oxidation, respectively, which is 12.68 times (MOR) and 14.67 times (EOR) higher than that of commercial Pd/C. This is probably attributed to the cage-like structure of PdZn/NC separating the Pd nanoclusters , resulting in high Pd dispersion. Simultaneously, the electronic property of Pd is adjusted after the formation of the complete PdZn alloy, improving the desorption of the carbon-based intermediates from the Pd active sites. This increases the CO poisoning resistance, resulting in good alcohol electrocatalytic oxidation activity and stability.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2017
·
IF 6.844
Lingfeng Shen,Shanjun Mao,Jianqing Li,Mingming Li,Ping Chen,Haoran Li,Zhirong Chen,Yong Wang
This work highlights a novel hybrid catalyst, intermetallic PdZn on CN@ZnO (PdZn/CN@ZnO), which serves as a highly efficient heterogeneous catalyst for semihydrogenation of 2-methyl-3-butyn-2-ol utilizing water as the solvent. Compared with intermetallic PdZn on ZnO (PdZn/ZnO), PdZn/CN@ZnO displays almost sixfold higher TOF while retaining high selectivity. It is assumed that the introduction of biomass-derived hydrophilic nitrogen-doped carbon into the ZnO helped to promote catalyst dispersion in aqueous media, ensuring better mass transfer. Further experiments and theoretical calculations showed that from Pd particles to intermetallic PdZn, the decrease of corner and edge Pd atoms might be a factor leading to the improvement of selectivity. Recycling experiments demonstrated that the PdZn/CN@ZnO catalyst could be reused at least eight times without significant decrease in activity or selectivity. Furthermore, when applied to industrially relevant alkenols that are building molecules for the production of vitamin E, the present catalyst still offered excellent performance. It is expected that the present catalytic system will demonstrate its high potential for practical production of vitamin E.
研究领域:
催化化学
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材料科学
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有机合成
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2018
·
IF 11.698
Yazhi Yin,Bing Hu,Xinliang Li,Xiaohai Zhou,Xinlin Hong,Guoliang Liu
Direct CO 2 hydrogenation to methanol provides a means of CO 2 fixation and a way of hydrogen storage in a more energy-dense and transportable form. Pd-ZnO catalysts can be active for this reaction, but their activities are strongly associated with the preparation methods which influence the dispersion and stability of Pd nanoparticle. Here we report a novel fabrication of highly effective PdZn alloy catalysts derived from Pd@zeolitic imidazolate framework (ZIF-8) for the hydrogenation of CO 2 . The confinement of subnanometric Pd particles in the pore framework of ZIF-8 facilitates the formation of Pd-ZnO interfaces with strong-metal-support-interaction (SMSI) after a simple pyrolysis under air condition. The porous texture and high surface area of ZnO ensures a high dispersion of Pd nanoparticles. Different pyrolysis temperatures were studied in catalysis and the highest methanol yield reached 0.65 g g cat −1 h −1 at 270 °C, 4.5 MPa, with a TOF of 972 h −1 , over a PdZn catalyst prepared at 400 °C. Such excellent activity has ranked the top reported values over advanced Pd-based catalysts under comparable conditions. The crucial factors for such high methanol yield are the formation of small-sized PdZn alloy particles after H 2 reduction and abundant surface oxygen defects on ZnO. The SMSI between PdZn and ZnO also ensures a long term stability of our PdZn catalysts. At last, we propose the active site that was strongly associated with methanol formation is a PdZn alloy rather than metallic Pd.
研究领域:
催化化学
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Xing Yan,Dongren Cai,Meihong Lin,Zhijie Wu,Yegang Xia,Yanmei Cai,Sajid Ali,Kok Bing Tan,Andriambinintsoa Ranaivoson Tojonirina,Hao Sun,Guowu Zhan
The selective hydrogenation of CO 2 to methanol demands precise control of both catalyst architecture and reaction pathways. Here, we design an atomic layer deposition (ALD)-engineered Pd/ZnO/ZrO 2 ternary catalyst with atomic-scale ZnO interlayers to decouple and reconfigure active sites at dual interfaces (Pd-ZnO and ZnO-ZrO 2 ). This interfacial engineering drives a 7-fold enhancement in methanol space–time yield (0.584 vs. 0.084 g MeOH g cat −1 h −1 ) and switches the dominant reaction pathway from CO-mediated to formate-driven selectivity (methanol selectivity remarkably surges from 6 % to 64 %). Multimodal characterization and theoretical calculations reveal that ZnO interlayers orchestrate bifunctional cooperation: activating CO 2 /CO adsorption while suppressing CO/CH 4 formation through electronic effects. Long-term stability study uncovers a dynamic restructuring mechanism, where Pd-ZnO interfaces gradually evolve into PdZn β alloy phases under the reaction conditions. This work establishes ALD-mediated interface design as a generalizable strategy to manipulate reaction networks and methanol selectivity in catalytic CO 2 hydrogenation systems.
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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可持续能源
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表面科学
✓ 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）