JOURNAL OF CATALYSIS
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2021
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IF 7.92
Xixi Liu,Yanxin Wang,Bo Li,Bing Liu,Wei Wang,Nian Xiang,Zehui Zhang
The catalytic acceptorless dehydrogenation of primary amines into imines and H 2 represents one of the most important organic transformations, and the in-situ utilization of the generated H 2 for chemical reduction reactions has never been reported in previous research. Herein, nitrogen-doped carbon supported nickel catalysts (abbreviated as Ni/NC-T, where T represents the pyrolysis temperature) were facilely prepared by the simple pyrolysis process, and the Ni/NC-600 catalyst demonstrated excellent catalytic performance towards the tandem reaction of the dehydrogenation of primary amines into imines and the subsequent hydrodeoxygenation of sulfoxides into sulfides using the in-situ released H 2 , affording high to quantitative yields. The developed methods demonstrated some advantages such as the use of heterogeneous non-noble metal catalysts with low cost and high stability, and the in-situ utilization of generated H 2 with high atom efficiency.
研究领域:
有机化学
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催化化学
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产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
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IF 3.9
Junpeng He,Ruiqing Zhang,Xi Chen,Bofeng Zhang,Guozhu Liu
Active fuel cooling is an effective way to overcome the thermal barrier for hypersonic flight. Pt-based nanofluid catalysts are effective in enhancing the chemical heat sink of endothermic hydrocarbon fuels (EHFs) by facilitating a catalytic dehydrogenation-cracking reaction. However, highly-dispersed Pt nanoparticles often face the problem of poor thermal stability in nanofluids. In this work, a NaH-assisted deprotonation method was applied to synthesize N-heterocyclic carbene (NHC)-capped highly-dispersed Pt nanoparticles (Pt@NHC14). The average size of the Pt nanoparticles in optimized Pt@NHC14 was 2.4 nm. Pt@NHC14 exhibited a high heat sink of 3.80 MJ/kg at 725 °C in the quasi-homogeneous conversion of decalin, which was 10% higher than Pt@ILs14 without a deprotonation strategy. This could be ascribed to the dehydrogenation process being promoted, which was verified by a hydrogen yield of 9.5% on highly dispersed Pt of Pt@NHC14, and that is 46% higher than that of Pt@ILs14. This research synthesizes N-heterocyclic carbene-capped highly-dispersed Pt nanoparticles and provides valuable insights into the strong endothermic technology.
研究领域:
材料科学
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化学工程
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航空航天工程
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Changgui Wu,Mengke Xu,Feifei Song,Biao Ma,Fuling Li,Chengxiang Shi,Zhen-Feng Huang,Ruijie Gao,Xiangwen Zhang,Lun Pan,Ji-Jun Zou
Monobenzyltoluene (H0-BT) is a promising liquid organic hydrogen carrier (LOHC), and continuous reaction process represents a more favorable approach in the large-scale hydrogen storage. In this work, the impacts of Pt loading and reaction conditions on the dehydrogenation performance of perhydro-monobenzyltoluene (H12-BT) over Pt/Al 2 O 3 were conducted in a fixed-bed reactor. The results indicate that the dehydrogenation activity of catalyst shows a volcano type as increasing Pt loading, reaching a maximum at 3 wt%. 1 wt% Pt loading is the most appropriate in consideration of the dehydrogenation activity and hydrogen purity. High reaction temperature and low pressure can facilitate dehydrogenation kinetics but result in the undesired byproducts, therefore, the optimal reaction conditions are 320 °C and 0.7 MPa. Additionally, the dehydrogenation performance of H12-BT and perhydro-dibenzyltoluene (H18-DBT) were compared under the similar conditions, revealing that H12-BT may be a superior hydrogen storage carrier.
研究领域:
化学工程
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能源科学
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2016
·Vol. 41
·期 15
·6362-6368
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IF 3.205
Di-Chang Zhong,Yue-Lei Mao,Xin Tan,Ping Zhong,Liang-Xian Liu
Chemical hydrogen storage, endowed with superiorities of safety and efficiency, has been regarded as one of the most promising approaches. The design and synthesis of metallic catalytic system is an key step for development of chemical hydrogen storate materials. In this paper, we report that RhNi nanocatalyst, formed by spontaneously alloying of well-dispersed Rh and Ni NPs , exhibits much higher performance in the catalytic dehydrogenation of hydrous hydrazine.
研究领域:
材料化学
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催化化学
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纳米科学
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能源化学
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氢能源
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DOI
高影响因子
CATALYSIS LETTERS
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2021
·Vol. 152
·期 6
·1711-1718
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IF 3.186
Wu Shaohua,Su Tongtong,Liu Senqun,Cheng Dan,Zeng Rong,Ma Xiaohua,Liang Sanqi,Ding Shunmin,Chen Chao
Developing an ideal stabilizer to prevent the aggregation of nanoparticles is still a big challenge for the practical application of noble metal nanocatalysts. Herein, we develop a charge (NTf 2 − ) modified porous organic polymer (POP-NTf 2 ) to stabilize ultrasmall platinum nanoparticles. The catalyst is characterized and applied in the catalytic dehydrogenative coupling of silanes with alcohols. The catalyst exhibits excellent catalytic performance with highly dispersed ultrasmall platinum nanoparticles (ca. 2.22 nm). Moreover, the catalyst can be reused at least five times without any performance significant loss and Pt NPs aggregation. Graphic Abstract
研究领域:
材料科学
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催化化学
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DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2018
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IF 4.229
Bin Wang,Tie-yan Chang,Zhao Jiang,Jin-jia Wei,Yong-hai Zhang,Sen Yang,Tao Fang
Through systematical experiments, a comparative study was conducted concerning several graphene-supported noble metal catalysts for dehydrogenation of dodecahydro-N-ethylcarbazole (12H-NEC). It was found that the catalytic activity of the prepared graphene-supported noble metal catalysts was following the order of Pd > Pt > Rh > Ru > Au for the dehydrogenation process. Pd supported on reduced graphene oxide (rGO) prepared by one-pot in situ synthesis has much more excellent catalytic performance than other kinds of catalysts investigated for comparison, simultaneously the using amount of noble metals can obviously be decreased. To be specific, at 453 K, the final dehydrogenation product catalyzed by the novel catalyst of Pd/rGO is N-ethylcarbazole (NEC) and the process selectivity was increased from 44.77% (commercial Pd/Al 2 O 3 ) to 97.65%, as well as the dehydrogenation ratio reached 99.14%. In addition, the novel catalyst is also superior to other reported catalysts in terms of dehydrogenation performance of 12H-NEC. Its dehydrogenation activity at 443 and 433 K of Pd/rGO was tested and the catalytic performance keeps stable at the two temperatures. Based on the experimental data, kinetic calculation was carried out and some fundamental parameters regarding reaction kinetics was obtained.
研究领域:
化学工程
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材料科学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Shiyao Lu,Jian Zhang,Hao Meng,Xiaoyuan Qin,Jianbin Huang,Yehao Liang,Feng-Shou Xiao
The direct dehydrogenation of ethyl lactate (EL) to produce ethyl pyruvate (EP) over non-precious heterogeneous catalysts is highly desirable, but challenging. Herein, we report a highly efficient silica-supported copper catalyst prepared via a hydrolysis-precipitation method (Cu/SiO 2 -HP) for the dehydrogenation of ethyl lactate, which exhibited an 85.4 % EL conversion with 91.1 % selectivity toward EP at 320 °C. XAFS, in situ XPS, and CO-adsorption FT-IR spectra revealed that the Cu/SiO 2 -HP catalyst had abundant Cu 0 /Cu + interfaces. In situ FT-IR spectra, kinetic studies , and theoretical calculations also demonstrated that the Cu 0 /Cu + interfaces synergistically activate the O−H and C−H bonds in the adsorbed EL for direct dehydrogenation into EP. The H/D kinetic isotope effect for model reaction confirmed that C−H bond activation is the key step in the dehydrogenation reaction. This study offers a new approach toward the selective conversion of EL into EP, which is of great significance for biomass conversion .
研究领域:
催化
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化学工程
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材料科学
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生物质转化
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产品关联
DOI
高影响因子
Catalysis Science & Technology
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2021
·Vol. 11
·期 15
·5250-5259
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IF 6.119
Zhiyang Zhang,Wenlong Xu,Xiaomei Ye,Yonglan Xi,Cunpu Qiu,Liping Ding,Gui Liu,Qingbo Xiao
Enclosing metal clusters in zeolites can enhance their catalytic performance due to the complex effects of the zeolitic environment. However, for the first time, herein, we report the significant passivation effects of the surrounding zeolitic framework on the d-band center and catalytic performance of enclosed Pt clusters. For the dehydrogenation of propane to propylene, the Pt/NaX catalyst with Pt clusters on the exterior of X-zeolite showed a ∼1100% enhancement in TOF and largely improved selectivity for propylene compared with the corresponding Pt@NaX catalyst, in which the Pt clusters were stuck to the inside of X-zeolite. Moreover, less coke deposition and high stability were detected in Pt/NaX after the reaction for 18 h. Combining the detailed experiments and DFT calculations, it was revealed that the significant passivation effect is mainly attributed to the surrounding zeolitic framework for the enclosed Pt clusters, which decreases the d-band center of the Pt clusters and weakens the activation of propane, preventing the desorption of propylene with a reduction in propylene selectivity and increase in coke deposition. Thus, the present investigation reveals that enclosing metal clusters in zeolites may not be beneficial for some specific catalytic reactions, deepening the understanding for this type of catalyst of metal clusters enclosed in zeolites.
研究领域:
催化
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化学工程
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材料科学
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物理化学
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Qianlin Zhang,Zhao Zhang,Yueer Ma,Wenchen Ren,Xiaomin Dai,Hui Chang,Xunjin Zhu
A series of Pt/CeO 2 compounds with hollow spheres (Pt/CeO 2 –S), wires (Pt/CeO 2 –W), and particle (Pt/CeO 2 –P) morphologies were prepared and further used for catalytic liquid organic hydrogen carrier (LOHC) dehydrogenation. The exposure and distribution of different crystal faces affected the nucleation process of crystals and then formed different microscopic morphologies. Compared with Pt/CeO 2 –W and Pt/CeO 2 –P, Pt/CeO 2 –S showed hollow spherical structures with significantly higher oxygen vacancy concentrations and specific surface areas. These structural differences not only affected platinum (Pt) dispersion, but also affected the activity and stability of the catalyst, thus promoting methylcyclohexane (MCH) conversion. The fixed bed reaction showed that Pt/CeO 2 –S had excellent catalytic activity, with the MCH conversion rate at 97.7 % and hydrogen release rate of 350.50 mmol/g (Pt) /min, and it still maintained stable activity after 72 h. Under the same conditions, the MCH conversion rates for Pt/CeO 2 –W and Pt/CeO 2 –P were only 77.23 % and 32.02 %, respectively. Therefore, through the growth pattern and morphology controls of catalyst supports, this was an effective means for improving the dehydrogenation performance of LOHC.
研究领域:
催化
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化学工程
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材料科学
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产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
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2024
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IF 15.7
Mengzhen Ren,Tianfu Liu,Yuanyuan Dong,Zheng Li,Jiaxin Yang,Zhenheng Diao,Hongjin Lv,Guo-Yu Yang
ABSTRACT Simultaneously harnessing the photogenerated electrons and holes to convert thiols into the value-added disulfides with the concomitant formation of H 2 represents a highly promising strategy for maximizing the conversion of solar energy into chemical energy. Herein, we report an effective catalytic system comprising CdS nanorods (NRs) and Ni-containing polyoxometalate (Na 6 K 4 [Ni 4 (H 2 O) 2 (PW 9 O 34 ) 2 ] (Ni 4 P 2 )) (Ni 4 P 2 /CdS), which exhibited efficient photocatalytic activities towards the near-unity dehydrocoupling of 4-methoxythiophenol (4-MTP) into disulfide and H 2 evolution. The photooxidative dehydrocoupling of 4-MTP can be finished after 4 h photocatalysis , leading to 98.39% conversion of 4-MTP with the yield of disulfide and H 2 reaching 24.45 and 25.96 μmol, respectively. The Ni 4 P 2 /CdS catalytic system also showed good photocatalytic recycling stability. Comprehensive experimental and characterization results indicated that the synergistic cooperation between CdS NRs and Ni 4 P 2 facilitated the separation and migration of the photogenerated electron-hole pairs, thereby improving the photocatalytic dehydrocoupling of 4-MTP to disulfide coupling with hydrogen production .
研究领域:
化学
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材料科学
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催化
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太阳能转换
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）