Science China-Materials
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2022
·Vol. 66
·期 1
·169-178
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IF 8.64
Wei Haisheng,Song Huaxing,Ren Yujing,Yan Xiaorui,Fang Geqian,Wang Wenhua,Ren Wanzhong,Zhu Mingyuan,Lin Jian
Metal-organic frameworks (MOFs) derived Co-based catalysts have received extensive attention in the chemoselective hydrogenation of nitroarenes, while they usually require a lot of solvent during the synthesis and identification of active species. This study explores a solid-phase synthesis strategy to obtain MOF precursors without using any solvent, which is then foamed and pyrolyzed to synthesize the Co@NC-X catalyst. It was found that a nitrogen-doped graphene shell can well encapsulate the Co nanoparticles. The resulting catalyst, which was pyrolyzed at 800°C, exhibited ~100% conversion for the hydrogenation of 3-nitrostyrene and >99% selectivity to 3-vinylaniline. This catalyst also showed excellent stability and good substrate universality for the hydrogenation of extensive substituted nitroarenes. Various characterizations revealed a positive relationship between the catalytic performance and the content of Co—N species tuned by pyrolysis temperature. This work provides a novel and green strategy to design an efficient Co-based catalyst for chemoselective hydrogenation.
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JOURNAL OF CATALYSIS
·
2022
·
IF 8.047
Lihua Zhu,Huan Zhang,Huaze Zhu,Huan Fu,Anna Kroner,Zhiqing Yang,Hengqiang Ye,Bing Hui Chen,Rafael Luque
Herein, we report a simple synthesis of PtNiCo trimetallic nanoparticles (NPs) loaded on carbon black (PtNiCo/C) via ambient-temperature chemical reduction and galvanic replacement reaction. The influence of thermal treatment temperature in 10 %H 2 /N 2 on PtNiCo NPs in PtNiCo/C-X nanostructures is revealed, where, X = 200 °C, 500 °C. XRD, XPS, TEM, HAADF-STEM, HRTEM, STEM-EDX elemental line-scanning (mapping), HS-LEIS, H 2 -TPR, atomic resolution aberration-corrected STEM (AC-STEM), XANES and EXAFS have been employed to characterize various nanostructures of PtNiCo NPs in PtNiCo/C-X. We established the relationship of nanostructure-reducing temperature thus catalytic behavior of PtNiCo/C-X: PtNiCo/C-200 ∼ Pt island (single atom and cluster)-on-NiCo alloy NP, PtNiCo/C-500 ∼ PtNiCo alloy NPs. PtNiCo/C-200 provides much improved catalytic activity and selectivity to target products ( NO 2 group hydrogenation) as compared to PtNiCo/C-500 for nitroarenes selective hydrogenation under mild reaction conditions (1.0 MPa-H 2 pressure, 18 °C or 40 °C-reaction temperature). That is considered to be closely correlated with the synergy effect of Pt islands and NiCo alloy nanoparticles in PtNiCo/C-200.
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ACS Catalysis
·
2021
·
IF 13.084
Muhong Li,Shanyong Chen,Qike Jiang,Qingliang Chen,Xuan Wang,Yong Yan,Jian Liu,Changchang Lv,Weiping Ding,Xuefeng Guo
The production of functionalized anilines by chemoselective hydrogenation of nitroarenes occupies an important position in the chemical industries. Recently, cobalt and nitrogen codoped carbon (Co–N–C) catalysts have been reported to show outstanding catalytic performance in this process, whereas the nature of their active sites is still at the center of intense debate. In this paper, based on the well-controlled experiments on four types of typical Co–N–C materials derived from different methodologies, several unusual generalities in the hydrogenation of nitroarenes are clearly revealed, including protic-solvent dependence, antipoisoning, acid resistance, and reversible deactivation. Further investigations indicate that the single-atom species Co–Nx are the main active sites of the Co–N–C catalysts in this chemoselective hydrogenation process. The present work sheds light on the mechanism study on the metal–N–C catalysts and further contributes to the rational design of the high-performance single-atom catalysts.
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Nature Communications
·
2020
·Vol. 11
·期 1
·1-8
·
IF 12.121
Du Xiaorui,Huang Yike,Pan Xiaoli,Han Bing,Su Yang,Jiang Qike,Li Mingrun,Tang Hailian,Li Gao,Qiao Botao
The strong metal-support interaction (SMSI) has long been studied in heterogonous catalysis on account of its importance in stabilizing active metals and tuning catalytic performance. As a dynamic process taking place at the metal-support interface, the SMSI is closely related to the metal surface properties which are usually affected by the size of metal nanoparticles (NPs). In this work we report the discovery of a size effect on classical SMSI in Au/TiO 2 catalyst where larger Au particles are more prone to be encapsulated than smaller ones. A thermodynamic equilibrium model was established to describe this phenomenon. According to this finding, the catalytic performance of Au/TiO 2 catalyst with uneven size distribution can be improved by selectively encapsulating the large Au NPs in a hydrogenation reaction. This work not only brings in-depth understanding of the SMSI phenomenon and its formation mechanism, but also provides an alternative approach to refine catalyst performance.
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PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2018
·Vol. 42
·期 24
·19901-19907
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IF 3.201
Xin Wang,Yi-Fan Jiang,Ya-Nan Liu,An-Wu Xu
Because of the active components, ultra small size, and the strong metal–support interaction (SMSI) between the metal and the support, noble metal/support nanocatalysts show high catalytic activity in chemical and photochemical reactions. Palladium is one of the most extensively used noble metals due to its outstanding properties. However, the high price and the trend of aggregation are two obvious defects which prevent further application of palladium in large-scale synthesis. Herein, we chose a novel oxide component Er2O3 which can effectively reduce the aggregation of palladium nanoparticles as the support. Thus, a series of highly efficient Er2O3 nanocatalysts with low palladium loading (ranging from 1.25 wt% to 2.25 wt%) were prepared as highly efficient hydrogenation nanocatalysts. Notably, the 1.75 wt% Pd–Er2O3 achieved a remarkable turnover frequency (TOF) value of 9013 h−1 for the hydrogenation of styrene at room temperature and 1 atm H2. The sample can also catalyze the hydrogenation of a variety of functional nitroarenes with excellent catalytic properties using H2 as the reductant, which was probably attributed to the synergistic effect of the strong metal–support interaction (SMSI) and strong chemisorption of H2 on Pd–Er2O3. This work could provide a new strategy and inspiration to prepare noble metal particles loaded on oxide supports with remarkable catalytic performance for various chemical transformations.
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FUEL
·
2024
·
IF 6.7
Jing Li,Xiaorui Yan,Yujing Ren,Tiantian Liu,Kairui Li,Haisheng Wei
Design of metal Co-based catalysts by different strategies has aroused many attentions in the chemoselective hydrogenation of nitroarenes to improve their catalytic performance. Herein, Co(6)-N-C catalyst with highly dispersed metal Co and Co-N species was synthesized by the assistance of formed Zn species, which exhibits better performance than single atom Co catalyst in the selective hydrogenation of 3-nitrostyrene, in which the increasing of hydrogenation activity is usually accompanied by unsatisfactory selectivity. In this work, Co(6)-N-C catalyst obtains 98.5 % conversion and > 99 % selectivity of 3-vinylaniline, as well as excellent cyclic stability and desirable substrate universality for the hydrogenation of other substituted nitroarenes. It is demonstrated that the good performance is ascribed to the synergy of metallic Co and Co-N species in the Co(6)-N-C catalyst, improving the activity and selectivity. This work provides a novel strategy to construct an efficient Co-based catalyst for enhanced hydrogenation performance.
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