Single-site catalyst promoters accelerate metal-catalyzed nitroarene hydrogenation

Wang, Qianqian; Guan, Erjia; Zhang, Jian; Yang, Jun; Zhu, Yihan; Han, Yu; Yang, Ming; Cen, Cheng; Fu, Gang; Gates, Bruce C.; Xiao, Feng‐Shou

doi:10.1038/s41467-018-03810-y

Cited by 174 publications

(124 citation statements)

References 35 publications

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“…It was reported that these bonds strongly influence the catalytic properties in hydrogenations. 44 To exclude the effect of Sn-O-Si bonds, we prepared carbon-supported PtSn/C iNPs and tested their catalytic performance for the acetylene semi-hydrogenation. As shown in Figure 6E, the selectivity of PtSn/C showed a similar trend as PtSn@mSiO2, indicating that the effect of Sn-O-Si bonds, if any, is less dominant.…”

Section: Discussionmentioning

confidence: 99%

Toward Phase and Catalysis Control: Tracking the Formation of Intermetallic Nanoparticles at Atomic Scale

Wang

Chen

et al. 2019

Chem

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Intermetallic nanoparticles (iNPs) have yielded enormous successes in catalytic applications by the formation of ordered phases. However, atomic level understanding of the alloying mechanism, which plays a pivotal role for controlling intermetallic phases and tailoring their catalytic properties, is still elusive. In this study, we discovered a consecutive formation of ordered Pt3Sn and PtSn phases during the growth of Pt-Sn iNP inside a well-defined nano-reactor at elevated temperature using in-situ scanning transmission electron microscopy. We found that the surface-mediated diffusion of Sn controls overall dynamics of the reaction, while the unique coherent interfacial structure is determinative for the PtSn transformation. We then further controlled the phase selection of Pt-Sn iNPs and demonstrated their distinguishable catalytic behaviors. Our findings not only provide detailed experimental evidence on the alloying mechanism in intermetallic nanoscale systems, but also pave the way for mechanistic control of synthesis and catalytic properties of iNPs. SUMMARYIntermetallic nanoparticles (iNPs) have yielded enormous successes in catalytic applications by the formation of ordered phases. However, atomic level understanding of the alloying mechanism, which plays a pivotal role for controlling intermetallic phases and tailoring their catalytic properties, is still elusive. In this study, we discovered a consecutive formation of ordered Pt3Sn and PtSn phases during the growth of Pt-Sn iNP inside a well-defined nanoreactor at elevated temperature using in-situ scanning transmission electron microscopy. We found that the surface-mediated diffusion of Sn controls overall dynamics of the reaction, while the unique coherent interfacial structure is determinative for the PtSn transformation. We then further controlled the phase selection of Pt-Sn iNPs and demonstrated their distinguishable catalytic behaviors. Our findings not only provide detailed experimental evidence on the alloying mechanism in intermetallic nanoscale systems, but also pave the way for mechanistic control of synthesis and catalytic properties of iNPs.

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Section: Discussionmentioning

confidence: 99%

Toward Phase and Catalysis Control: Tracking the Formation of Intermetallic Nanoparticles at Atomic Scale

Wang

Chen

et al. 2019

Chem

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“…Modifying the electron density of the nanoparticles via the corresponding supports is an alternative strategy . In a recent report, Xiao and co‐workers introduced Au, Pt or Ni nano particles on the support of TiO 2 with the single atom dispersed Sn, and the Sn−O−Ti provide oxygen vacancies to enhance the selectivity . Su et al.…”

Section: Introductionmentioning

confidence: 89%

Rh Catalyzed Selective Hydrogenation of Nitroarenes under Mild Conditions: Understanding the Functional Groups Attached to the Nanoparticles

Tian

Zhou

et al. 2019

ChemCatChem

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Modifying the surface of metal catalyst is a crucial subject for improving the heterogeneous metal catalysts. It is still a great challenge to understand the structure‐activity relationship (SAR) between the surface supporting groups and the metal particles. Herein, Rh NPs supported on the magnetic silica sphere with various functional groups (−NH2, −SH, −SO3H, −N=CH2, −Cl, −NHCOCH3 and −NHCH2Ph) have been prepared for catalytic hydrogenation of nitroarenes under atmospheric pressure at room temperature. We discover that the chemical state of Rh NPs depends on the supporting groups significantly. The electron‐donating functionalities can effectively elevate the Rh0/Rh3+ ratio, which increase the catalytic performance both in conversion and selectivity. The amino group decorated catalyst has such a good selectivity that no dechlorination reaction is observable in the hydrogenation of 2‐chloro‐3‐nitropyridine. What's more, by introducing magnetic Fe3O4 nuclei and mesoporous silica encapsulating layer, the catalyst can be recovered conveniently by an external magnet, and can be reused 10 cycles without any loss of activity.

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“…The Raman spectra (Figures S5) of as‐made samples indicate that the Pd loading can significantly decrease the surface defect of carbon supports which is the same case for Pd/CNTs. The reason for this could be that the O atoms on the carbon surface are responsible for holding the metal component . It can be concluded that the carbon supports promote the Pd 2+ reduction, and the Pd size and distribution are affected by surface properties of carbon supports.…”

Section: Figurementioning

confidence: 99%

Low‐Temperature Fast Production of Carbon and Acetic Acid Dual‐Promoted Pd/C Catalysts

Yao

Chen

et al. 2019

Chemistry A European J

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The Pd/C catalysts are widely used in synthesis of fine chemicals in industry, but their production suffers from a complicated two‐step process involving impregnation and reduction, and requires large amounts of solvents and reductant, which would lead to a series of issues such as time consumption, resource waste and environmental pollution. Herein, ultra‐small Pd nanoparticles uniformly anchored on carbon nanotubes (Pd/CNTs) were synthesized by using a one‐pot and low‐temperature reduction strategy. The present process/technology is very sensitive to and controlled by the supports and solvents, and the carbon support and acetic acid synergistically play crucial and decisive roles in the fast production of Pd/C catalysts. Also, the used solvents can be recycled and reutilized, which meets the requirements of sustainable chemistry and green economy. When the as‐obtained Pd/CNTs catalyst was used to catalyze the oxidation of benzyl alcohol to benzaldehyde, it achieved a conversion efficiency as high as 99.3 % and a high selectivity up to >99.9 %. The simple, scalable and environmentally friendly strategy can be extended to anchor Pd nanoparticles on various carbon substrates, which sheds a new light on the synthesis of Pd/C catalysts.

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Single-site catalyst promoters accelerate metal-catalyzed nitroarene hydrogenation

Cited by 174 publications

References 35 publications

Toward Phase and Catalysis Control: Tracking the Formation of Intermetallic Nanoparticles at Atomic Scale

Toward Phase and Catalysis Control: Tracking the Formation of Intermetallic Nanoparticles at Atomic Scale

Rh Catalyzed Selective Hydrogenation of Nitroarenes under Mild Conditions: Understanding the Functional Groups Attached to the Nanoparticles

Low‐Temperature Fast Production of Carbon and Acetic Acid Dual‐Promoted Pd/C Catalysts

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