Hollow carbon anchored highly dispersed Pd species for selective hydrogenation of 3-nitrostyrene: metal-carbon interaction

Lou, Yang; Xu, Jia; Wu, Honglu; Liu, Jingyue

doi:10.1039/c8cc07430e

Cited by 25 publications

(17 citation statements)

References 50 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…The geometric and electronic properties of active metal species play a crucial role in determining the adsorption behavior of functional groups and the dissociation behavior of H 2 ( Armbrüster et al., 2012 , Blaser et al., 2009 , Wei et al., 2014 , Wei et al., 2017b , Lou et al., 2018 ). Pt metals show excellent catalytic capability of H 2 dissociation with a reaction barrier as low as 0 and 0.067 eV on Pt (001) and Pt (111) surfaces, respectively ( Pasteur et al., 1997 , Olsen et al., 1999 ).…”

Section: Resultsmentioning

confidence: 99%

Nanocarbon-Edge-Anchored High-Density Pt Atoms for 3-nitrostyrene Hydrogenation: Strong Metal-Carbon Interaction

Lou

Liu

2019

iScience

Self Cite

View full text Add to dashboard Cite

SummaryStrong metal-support interaction (SMSI) has been widely used to improve catalytic performance and to identify reaction mechanisms. We report that single Pt atoms anchored onto hollow nanocarbon (h-NC) edges possess strong metal-carbon interaction, which significantly modifies the catalytic behavior of the anchored Pt atoms for selective hydrogenation reactions. The strong Pt-C bonding not only stabilizes single Pt atoms but also modifies their electronic structure, tunes their adsorption properties, and enhances activation of reactants. The fabricated Pt1/h-NC single-atom catalysts (SACs) demonstrated excellent activity for hydrogenation of 3-nitrostyrene to 3-vinylaniline with a turnover number >31,000/h, 20 times higher than that of the best catalyst for such selective hydrogenation reactions reported in the literature. The strategy to strongly anchor Pt atoms by edge carbon atoms of h-NCs is general and can be extended to construct strongly anchored metal atoms, via SMSI, onto surfaces of various types of support materials to develop robust SACs.

show abstract

Section: Resultsmentioning

confidence: 99%

Nanocarbon-Edge-Anchored High-Density Pt Atoms for 3-nitrostyrene Hydrogenation: Strong Metal-Carbon Interaction

Lou

Liu

2019

iScience

Self Cite

View full text Add to dashboard Cite

show abstract

“…639 Interestingly, electron-deficient Pd NP deposited on highly defective carbon support were reported to be more active and more selective for the hydrogenation of 3-nitrostyrene to 3-ethylnitrobenze than Pd NP on CB. 640 For the reduction of o-nitroaniline to 1,2-benzenediamine on Au NP of different size (5-40 nm) deposited on GO, the electrons are better transferred from GO (higher work function) to Au NP (lower work function) when the Au NP size decreases. 421 The larger charge transfer from GO to the smaller Au NP leads to a higher catalytic activity, since the enhanced electron transfer should promote the hydrogen dissociation on the Au NP surface.…”

Section: Ag8/n-gmentioning

confidence: 99%

A Theory/Experience Description of Support Effects in Carbon-Supported Catalysts

2019

View full text Add to dashboard Cite

Fermi level in vii) are shown in purple in ii)-vi) with an iso-value of ±0.003 a.u. Reprinted with permission from ref 57 . Copyright 2014 from the Royal Society of Chemistry; b) Molecular model of a corannulene-like element functionalized with three carboxylic groups from two different perspectives in the cpk representation (on the left). The final structure (190 elements in a cubic cell of 60 Å in size) obtained from random packing of the individual elements (on the right). Cyan: carbon, red: oxygen, white: hydrogen. Reprinted with permission from ref 59 Copyright 2017 from Elsevier; c) Side-views of Ru13 adsorbed on Gr-DV-2COOH site before (on left panel) and after a proton jump (right panel). C atoms are in black, O in red, H in with white and Ru in mocha. Reprinted with permission from ref 60 Copyright 2014 from Elsevier; and d) Spin-density projection in µB/a.u. 2 on the graphene plane around i) the hydrogen chemisorption defect (∆) and ii) the vacancy defect in the a sublattice. Carbon atoms corresponding to the a sublattice (o) and to the b sublattice (•) are distinguished. Simulated STM images of the defects are shown in iii) and iv), respectively. Reprinted with permission from ref 61 .

show abstract

“…This means that elemental Pd has a lower electron density, resulting in a lower surface energy. Thus, the surface of Au 3 Pd 1 NDs will prefer to adsorb and hydrogenate the groups of lower polarities, such as CC and CC groups, but hamper the hydrogenation to the higher polarity groups, such as nitro groups, making hydrogenation to unsaturated hydrocarbons preferential. , To support this opinion, the hydrogenation of a physical mixture of phenylacetylene and nitrobenzene over Au 3 Pd 1 NDs is also studied. As shown in Figures S14 and S15, at the initial stage, phenylacetylene is still preferentially hydrogenated in a stepwise pattern via styrene to phenylethane.…”

Section: Resultsmentioning

confidence: 99%

Au₃Pd₁ Nanodendrites with Hyperbranched Architectures: Green Synthesis at Room Temperature and Highly Selective Hydrogenation for 4-Nitrophenylacetylene

Yao

Zhao

et al. 2020

ACS Sustainable Chem. Eng.

View full text Add to dashboard Cite

Conceiving a simple, green, and mild one-pot route to grow and construct anisotropic bimetallic 3D architectures with multilevel structures and promising functions is highly desirable and technically important in many applications. Herein, a facile ionic liquid-modulated strategy is presented for the preparation of hyperbranched Au3Pd1 bimetallic nanodendrites (NDs) in aqueous solution at room temperature. To implement this protocol, HAuCl4 and Na2PdCl4 are used as precursors and ascorbic acid as a reductant, and a common ionic liquid 1-butyl-3-methylimidazolium chloride ([C4mim]Cl) is utilized to direct the anisotropic growth of 3D Au3Pd1 NDs, which exhibits an eco-friendly feature. It is shown that the alloy Au3Pd1 NDs possess multilevel architectures, that is, primary 3D large flowers (with diameters of about 2.5–4.0 μm), secondary 2D leaves, tertiary symmetric branches, and quaternary symmetric petals. A series of factors influencing morphologies and properties of the products are investigated, and the results indicate that both [C4mim]Cl and Au/Pd atomic ratios are crucial to the formation of 3D Au3Pd1 NDs. Owing to the well-defined morphology and probable electronic effects between Au and Pd, the 3D Au3Pd1 NDs display high catalytic selectivity and good durability toward stepwise hydrogenation of 4-nitrophenylacetylene with a 100% conversion and 99.5% selectivity to 4-nitrostyrene in the first step and then 100% conversion from 4-nitrostyrene and 96.7% selectivity to 4-nitroethylbenzene in the second step. It is believed that the well-defined 3D Au3Pd1 NDs would also exhibit promising applications in other catalysis and eletrocatalysis applications.

show abstract

Hollow carbon anchored highly dispersed Pd species for selective hydrogenation of 3-nitrostyrene: metal-carbon interaction

Abstract: Hollow nanocarbon supported Pd species are highly active (TOF of 21 845 h−1), selective (97%), and stable (4 cycles) for selective hydrogenation of 3-nitrostyrene to 3-ethylnitrobenze.

Cited by 25 publications

References 50 publications

Nanocarbon-Edge-Anchored High-Density Pt Atoms for 3-nitrostyrene Hydrogenation: Strong Metal-Carbon Interaction

Nanocarbon-Edge-Anchored High-Density Pt Atoms for 3-nitrostyrene Hydrogenation: Strong Metal-Carbon Interaction

A Theory/Experience Description of Support Effects in Carbon-Supported Catalysts

Au₃Pd₁ Nanodendrites with Hyperbranched Architectures: Green Synthesis at Room Temperature and Highly Selective Hydrogenation for 4-Nitrophenylacetylene

Contact Info

Product

Resources

About

Hollow carbon anchored highly dispersed Pd species for selective hydrogenation of 3-nitrostyrene: metal-carbon interaction

Abstract: Hollow nanocarbon supported Pd species are highly active (TOF of 21 845 h−1), selective (97%), and stable (4 cycles) for selective hydrogenation of 3-nitrostyrene to 3-ethylnitrobenze.

Cited by 25 publications

References 50 publications

Nanocarbon-Edge-Anchored High-Density Pt Atoms for 3-nitrostyrene Hydrogenation: Strong Metal-Carbon Interaction

Nanocarbon-Edge-Anchored High-Density Pt Atoms for 3-nitrostyrene Hydrogenation: Strong Metal-Carbon Interaction

A Theory/Experience Description of Support Effects in Carbon-Supported Catalysts

Au3Pd1 Nanodendrites with Hyperbranched Architectures: Green Synthesis at Room Temperature and Highly Selective Hydrogenation for 4-Nitrophenylacetylene

Contact Info

Product

Resources

About

Au₃Pd₁ Nanodendrites with Hyperbranched Architectures: Green Synthesis at Room Temperature and Highly Selective Hydrogenation for 4-Nitrophenylacetylene