Recent progress in heterogeneous metal and metal oxide catalysts for direct dehydrogenation of ethane and propane

Dai, Yihu; Gao, Xing; Wang, Qiaojuan; Wan, Xiaoyue; Zhou, Chunmei; Yang, Yanhui

doi:10.1039/d0cs01260b

Cited by 232 publications

(185 citation statements)

References 298 publications

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“…In the meantime, the heterogeneous catalyst systems have not only obtained the same rapid development but also attracted more and more attention. They not only have advantages in catalyst/product separation, no need for additives (acids, ligands, and salts), catalysts recyclability, reuse, etc., but also show comparable activity and product selectivity, which are very consistent with the goal of the atomic economy and sustainable development [25][26][27][28] . Shi and his co-workers 29 .…”

Section: Introductionsupporting

confidence: 69%

“…Surprisingly, the high steric substrate diphenylmethanamine could also be converted to the N, N-dimethyldiphenylmethanamine in a 72% yield. Moreover, the linear branched and cyclic aliphatic amines, furan, thiophene, pyrazole, and pyridine heterocyclic amines, which were previously reported challenging substrates [54][55][56] , were successfully converted to the corresponding N, N-di-methylated products in good to excellent yield (15)(16)(17)(18)(19)(20)(21)(22)(23)(24)(25)(26)(27)(28). The thin graphene layer encapsulated N-doping catalyst also showed very e cient reactivity and selectivity in the double dimethylation reaction of diamines (31).…”

Section: Resultsmentioning

confidence: 99%

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Facile synthesis of N-doped graphene encapsulated Pd@N/C catalyst and its efficient application in cascade flow synthesis of amines

Liu¹,

Sun²,

Song³

et al. 2021

Preprint

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N-methylamines, as an important class of chemicals, crucial building blocks, have been widely used in pharmaceutical companies and materials synthesis. Transition metal-catalyzed synthesis of N-methylamines, especially the heterogeneous catalyzed N-methylation of amines via different C1 sources has become the most promising methodology, due to the environmentally friendlier process and the recyclable and easily accessible catalysts. However, these reactions generally require activated toxic methyl iodide or dimethyl sulfoxide, and homogeneous catalysts or Raney nickel catalyst. The synthesis of amines still suffering from narrow scopes of amines, harsh reaction conditions, low selectivity of the desired products, and against the requirements of atomic economy and sustainable green environment. Herein, we developed a novel facile synthesis of nitrogen-doped graphene encapsulated Pd@NC nanocatalysts. The resulting heterogeneous catalyst was active for the synthesis of amines (more than 83 examples, yield up to 99%). The nitrogen-doped effect was unlike the previous report that poisoned the metal, it could increase the interaction with the active metal resulting in excellent stability. As far as we know, for the first time, the developed N-doped graphene encapsulated Pd@NC nanocatalyst showed excellent stability and activity of amines synthesis in the 20 times’ recycling test, industrially applicable flow reactor 2880 minutes’ test, and 99% purity of primary amine and tertiary amines product preparation test. Moreover, we have also shown the high atomic economy and environmentally friendlier tandem flow synthesis of N, N-dimethylamine products via the combination of reduction of nitrobenzene and N-methylation of amines, using the single one Pd@NC nanocatalyst with H2O as the only by-product. Upon our knowledge, this is a novel example of primary amine and tertiary amine synthesis methodology with the combined cascade reaction and flow process of nitrobenzene reduction and primary amines N-methylation with a single heterogeneous catalyst.

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Section: Introductionsupporting

confidence: 69%

Section: Resultsmentioning

confidence: 99%

Facile synthesis of N-doped graphene encapsulated Pd@N/C catalyst and its efficient application in cascade flow synthesis of amines

Liu¹,

Sun²,

Song³

et al. 2021

Preprint

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“…Furthermore, PDH is a structure-insensitive reaction, whereas, side reactions, such as hydrogenolysis, isomerization, and polymerization, are structure-sensitive reactions. [1][2][3] Moreover, since large Pt À Pt ensembles are well-known activators of undesired side reactions, the dilution of such ensembles (also known as the "ensemble effect") by alloying Pt with inactive metals such as Sn, [4][5][6] Ga, [7][8][9] In, [10] and Zn [11,12] has been generally applied to prevent side reactions. The ensemble effect can also be maximized by completely isolating the Pt atoms by the second metals, thus favoring the first and second C À H scissions, whereas the subsequent C À H scission would be successfully inhibited.…”

mentioning

confidence: 99%

Doubly Decorated Platinum–Gallium Intermetallics as Stable Catalysts for Propane Dehydrogenation

et al. 2021

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Propane dehydrogenation (PDH) is a promising chemical process that can satisfy the increasing global demand for propylene. However, the Pt-based catalysts that have been reported thus far are typically deactivated at ! 600 8C by side reactions and coke formation. Thus, such catalysts possess an insufficient life. Herein, we report a novel catalyst design concept, namely, the double decoration of PtGa intermetallics by Pb and Ca, which synergize the geometric and electronic promotion effects on the catalyst stability, respectively. Pb is deposited on the three-fold Pt 3 sites of the PtGa nanoparticles to block them, whereas Ca, which affords an electron-enriched single-atom-like Pt 1 site, is placed around the nanoparticles. Thus, PtGa À Ca À Pb/SiO 2 exhibits an outstandingly high catalytic stability, even at 600 8C (k d = 0.00033 h À1 , t = 3067 h), and almost no deactivation of the catalyst was observed for up to 1 month for the first time.

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“…Ethylene is one of the most important building blocks in chemical industry. Among its many uses is the production of ethylene via steam cracking [1] . This process is characterized by high energy consumption at temperatures >800 °C and suffers from adverse side reactions and severe coking [2] .…”

Section: Figurementioning

confidence: 99%

Electrochemical Oxidative Dehydrogenation of Ethane to Ethylene in a Solid Oxide Electrolyzer

Duan

Xie

2021

Angewandte Chemie

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Oxidative dehydrogenation of ethane to ethylene is an important process in light olefin industry; however, the over‐oxidation of ethane leads to low ethylene selectivity. Here, we report a novel approach to electrochemical oxidative dehydrogenation of ethane in anode in conjunction with CO2 reduction at cathode in a solid oxide electrolyser using a porous single‐crystalline CeO2 electrode at 600 °C. We identify and engineer the flux and chemical states of active oxygen species that evolve from the lattice at anode surface to activate and dehydrogenate ethane to ethylene via the reaction of epoxy species. Active oxygen species (O2−, O22− and O2−) at the anode surface effectively dehydrogenate ethane to ethylene, but O− species tend to induce deep oxidation. We demonstrate exceptionally high ethylene selectivity of 95 % and an ethane conversion of 10 % with a durable operation of 300 h.

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Recent progress in heterogeneous metal and metal oxide catalysts for direct dehydrogenation of ethane and propane

Abstract: Metal and metal oxide catalysts for non-oxidative ethane/propane dehydrogenation are outlined with respect to catalyst synthesis, structure–property relationship and catalytic mechanism.

Cited by 232 publications

References 298 publications

Facile synthesis of N-doped graphene encapsulated Pd@N/C catalyst and its efficient application in cascade flow synthesis of amines

Facile synthesis of N-doped graphene encapsulated Pd@N/C catalyst and its efficient application in cascade flow synthesis of amines

Doubly Decorated Platinum–Gallium Intermetallics as Stable Catalysts for Propane Dehydrogenation

Electrochemical Oxidative Dehydrogenation of Ethane to Ethylene in a Solid Oxide Electrolyzer

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