“…4 ). Among various modification strategies, the incorporation of different metals, especially the secondary active metals, into magnetic metal oxides has been shown to be effective in improving the catalytic performance [ 26 ]. Fig.…”
Section: Resultsmentioning
confidence: 99%
“…These heterogeneous catalysts showed good robustness and separability and had been used in industrial production, including fine chemical production. For the reduction of nitroaromatic compounds, doping of Pd has been reported to increase the catalytic activity of Fe 3 O 4 substances [ 26 ]. In particular, the synergistic effect between Pd and Fe has been shown to be effective in the catalysis of nitro aromatic hydrocarbons to corresponding amines [ 27 , 28 ].…”
Aniline is a group of important platform molecules that has been widely used in the synthesis of other high-value chemicals and pharmaceutical products. How to produce high-value anilines as the high-value chemical intermediates more efficiently and environmentally has always been a research topic in the industry. Catalytic hydrogenation is an environmentally friendly method for preparing halogenated anilines. Traditional noble metal catalysts face the problems of cost and noble metals residue. To improve the purity of the product as well as the activity and recyclability of the catalyst, we prepared a Pd/Fe magnetic bimetallic catalyst supported on N-doped carbon materials to reduce nitrobenzene to aniline under mild conditions. The catalyst has a low Pd loading of 2.35%. And the prepared bimetallic Pd/Fe@N/C catalyst showed excellent catalytic reactivity with the nitrobenzene conversion rate of 99%, and the aniline selectivity of 99% under mild reaction conditions of 0.8 MPa H
2
and 40 °C. A variety of halogenated and aliphatic nitro compounds were well tolerated and had been transformed to the corresponding target amine products with excellent selectivity. In addition, the novel N-doped graphene-encapsulated bimetallic magnetic Pd/Fe@N/C catalyst not only had magnetic physical properties, which was easy to separate, recover, and used for the recycling of the catalyst without metal leaching but also catalyzed highly selective reductive amination of aromatics was a green, economical and environmentally friendly reaction with the only by-product of H
2
O.
Graphical Abstract
Supplementary Information
The online version contains supplementary material available at 10.1007/s10562-023-04273-7.
“…4 ). Among various modification strategies, the incorporation of different metals, especially the secondary active metals, into magnetic metal oxides has been shown to be effective in improving the catalytic performance [ 26 ]. Fig.…”
Section: Resultsmentioning
confidence: 99%
“…These heterogeneous catalysts showed good robustness and separability and had been used in industrial production, including fine chemical production. For the reduction of nitroaromatic compounds, doping of Pd has been reported to increase the catalytic activity of Fe 3 O 4 substances [ 26 ]. In particular, the synergistic effect between Pd and Fe has been shown to be effective in the catalysis of nitro aromatic hydrocarbons to corresponding amines [ 27 , 28 ].…”
Aniline is a group of important platform molecules that has been widely used in the synthesis of other high-value chemicals and pharmaceutical products. How to produce high-value anilines as the high-value chemical intermediates more efficiently and environmentally has always been a research topic in the industry. Catalytic hydrogenation is an environmentally friendly method for preparing halogenated anilines. Traditional noble metal catalysts face the problems of cost and noble metals residue. To improve the purity of the product as well as the activity and recyclability of the catalyst, we prepared a Pd/Fe magnetic bimetallic catalyst supported on N-doped carbon materials to reduce nitrobenzene to aniline under mild conditions. The catalyst has a low Pd loading of 2.35%. And the prepared bimetallic Pd/Fe@N/C catalyst showed excellent catalytic reactivity with the nitrobenzene conversion rate of 99%, and the aniline selectivity of 99% under mild reaction conditions of 0.8 MPa H
2
and 40 °C. A variety of halogenated and aliphatic nitro compounds were well tolerated and had been transformed to the corresponding target amine products with excellent selectivity. In addition, the novel N-doped graphene-encapsulated bimetallic magnetic Pd/Fe@N/C catalyst not only had magnetic physical properties, which was easy to separate, recover, and used for the recycling of the catalyst without metal leaching but also catalyzed highly selective reductive amination of aromatics was a green, economical and environmentally friendly reaction with the only by-product of H
2
O.
Graphical Abstract
Supplementary Information
The online version contains supplementary material available at 10.1007/s10562-023-04273-7.
“…On the basis of results and recent reports, ,,,− the reduction process with the presence of CuNi-MOF catalysts and NaBH 4 includes (Figure a) (1) chemisorption of BH 4 – on the surface of the MOFs and (2) transfer electrons from BH 4 – to the reactants via the Cu and Ni sites states. The metal site states of MOF can effectively trap and accumulate long-lived electrons, and act as relay for the electrons transfer from BH 4 – to 4-NP, which is a crucial process in real catalytic systems.…”
mentioning
confidence: 76%
“…However, its reduction product 4-aminophenol (4-AP) is an important chemical and pharmaceutical intermediate . Currently, the reduction reaction from 4-NP to 4-AP is mostly catalyzed by novel metals. − The usage of novel metals has hindered the industrial application of the reduction product 4-AP. Furthermore, the novel metal particles (or the active sites) on the substrate surface easily fall off, resulting in poor stability and reusability.…”
mentioning
confidence: 99%
“…It is known that the reduction of 4-NP generally takes place on the surface of the catalysts. − There is an “induction time” of less than 5 s before the reduction of 4-NP as it needs time to absorb 4-NP onto the surface of the CuNi-MOFs and dissolve oxygen to react with NaBH 4 (Figure f) . The whole reaction is about 15 s (Figure f).…”
The design of efficient reduction catalysts is crucial
for sustainable
development in order to reduce waste and protect the environment.
Here, an ultrathin bimetallic metal–organic framework (MOF)
is synthesized and fabricated as an effective catalyst for the reduction
of 4-nitrophenol (which is harmful to the environment) to 4-aminophenol
(which is an important chemical and pharmaceutical intermediate).
The rapid reduction time of the as-prepared bimetallic CuNi-MOFs is
15 s, and the apparent rate constant is 0.153 s–1, which is far beyond the single-metal MOFs. Ultrafast transition
absorption spectra show that Cu doping can induce defect states, which
can effectively trap and store long-lived electrons in the catalytic
process. X-ray photoelectron spectra verify that Cu doping changes
the electron density distribution of CuNi-MOFs. It is believed that
the introduction of Cu sites leads to synergistic effects of Cu and
Ni sites, which significantly improves the catalytic activity of 4-NP.
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