Amorphous MoaZr0.8Ox-500 catalyzed selective oxidation of sulfides to sulfoxides mediated by 1O2 from direct heterolytic cleavage of H2O2 DOI
Tong Li,

Jiaheng Qin,

Xueyao Zhang

et al.

Inorganic Chemistry Frontiers, Journal Year: 2024, Volume and Issue: 11(23), P. 8411 - 8420

Published: Jan. 1, 2024

Sulfoxides, a class of pharmaceuticals and fine chemicals significant importance, are readily peroxidized to sulfones in the H 2 O system.

Language: Английский

Inducing Cu Charge Redistribution by Modulating Proximity with Zr(OH)4 for Selective Synthesis of Imines and Secondary Amines with Stoichiometric Benzyl Alcohol and Nitrobenzene DOI
Jie Song,

Chunxia Che,

Yiwei Dai

et al.

ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 1170 - 1181

Published: Jan. 6, 2025

The one-pot synthesis of amines from benzyl alcohol (BA) and nitrobenzene (NB) represents a step-economic method. However, reported works typically require more than 3 equiv BA to complete the transfer hydrogenation NB, few studies can achieve selective imines secondary amines. In our previous work, Zr(OH)4 demonstrated both dehydrogenation capabilities. Building on this, another component Cu was introduced enhance its catalytic performance for catalyzing coupling reaction between stoichiometric NB under H2 atmosphere. physical hybrid catalyst + selectively produced imines, while supported Cu/Zr(OH)4 yielded Characterization mechanism experiments revealed that modulating proximity leads (1) different adsorption abilities N-benzylideneaniline (NBA) (2) interactions in close contact, which stabilized electronic structure forming Cu+/Cu0 ion pairs with strong activation ability. This work presents design strategy offers an approach preparation N-benzylaniline.

Language: Английский

Citations

1
Zr(OH)4‐Catalyzed Semi‐Hydrogenation of Phenylacetylene with Terminal Zr‐O‐H as Active Site: Inactive for Free Styrene DOI

Wenxiang Wu,

Na Li,

Chunxia Che

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: July 24, 2024

Abstract In the field of industrial semi‐hydrogenation trace alkynes amidst alkene feedstocks, pivotal challenge lies in circumventing hydrogenation alkenes. Herein, we present Zr(OH) 4 as an innovative catalyst for phenylacetylene, demonstrating remarkable selectivity towards styrene (>96 %), while exhibiting inactivity free styrene. Notably, achieves a 95 % conversion quasi‐industry 1 mol phenylacetylene within styrene, with mere 0.44 loss. Experimental and theoretical results confirm both terminal Zr−O−H bridge can dissociate H 2 , plays crucial role on activating through sequential process C 6 5 C≡CH→C C=CH →C CH=CH . The high rate removal is attributed to its strong adsorption capacity, has significantly weaker capacity

Language: Английский

Citations

6
Zr(OH)4‐Catalyzed Semi‐Hydrogenation of Phenylacetylene with Terminal Zr‐O‐H as Active Site: Inactive for Free Styrene DOI

Wenxiang Wu,

Na Li,

Chunxia Che

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(42)

Published: July 24, 2024

Abstract In the field of industrial semi‐hydrogenation trace alkynes amidst alkene feedstocks, pivotal challenge lies in circumventing hydrogenation alkenes. Herein, we present Zr(OH) 4 as an innovative catalyst for phenylacetylene, demonstrating remarkable selectivity towards styrene (>96 %), while exhibiting inactivity free styrene. Notably, achieves a 95 % conversion quasi‐industry 1 mol phenylacetylene within styrene, with mere 0.44 loss. Experimental and theoretical results confirm both terminal Zr−O−H bridge can dissociate H 2 , plays crucial role on activating through sequential process C 6 5 C≡CH→C C=CH →C CH=CH . The high rate removal is attributed to its strong adsorption capacity, has significantly weaker capacity

Language: Английский

Citations

0
Physically hybrid Zr(OH)4 + CuO catalyzed selective aniline oxidation: A new Ph‐N˙$$ \dot{\mathbf{N}} $$OH mediated mechanism DOI

Jiaheng Qin,

Chong Liu,

Feng Zhao

et al.

AIChE Journal, Journal Year: 2024, Volume and Issue: 70(12)

Published: Aug. 27, 2024

Abstract Developing the sustainable and cost‐effective heterogeneous catalytic system for controlling chemoselectivity holds substantial importance in fine organic chemicals. Herein we construct a unique Zr(OH) 4 + CuO physically hybrid selective oxidation of anilines. alone leads to azoxybenzene formation, shifts reaction favorably toward nitrosobenzene. The proximity study indicates outperforms its counterparts synthesized through methods like ball‐milling, loading, coprecipitation, because closer exhibits stronger chemical interaction, restricting activity Zr‐OH hydroxyl sites. Through mechanistic experiments, situ DRIFT‐IR DFT calculations, new Ph‐OH intermediate mechanism is firstly proposed. Two self‐condensate form only , whereas could promote rapid transformation nitrosobenzene on hydrogen transfer process. Moreover, displays good recyclability robust scalability. This first report demonstrating utilization catalyst adjust selectivity aniline reaction.

Language: Английский

Citations

0
Amorphous MoaZr0.8Ox-500 catalyzed selective oxidation of sulfides to sulfoxides mediated by 1O2 from direct heterolytic cleavage of H2O2 DOI
Tong Li,

Jiaheng Qin,

Xueyao Zhang

et al.

Inorganic Chemistry Frontiers, Journal Year: 2024, Volume and Issue: 11(23), P. 8411 - 8420

Published: Jan. 1, 2024

Sulfoxides, a class of pharmaceuticals and fine chemicals significant importance, are readily peroxidized to sulfones in the H 2 O system.

Language: Английский

Citations

0