Pd@C core–shell nanoparticles on carbon nanotubes as highly stable and selective catalysts for hydrogenation of acetylene to ethylene

Zhang, Liyun; Ding, Yuxiao; Wu, Kuang‐Hsu; Niu, Yiming; Luo, Jingjie; Xia, Yang; Zhang, Bingsen; Su, Dangsheng

doi:10.1039/c7nr04992g

Cited by 38 publications

(24 citation statements)

References 26 publications

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“…As an important petrochemical raw material, ethylene is currently produced by cracking hydrocarbon from petroleum feedstock such as naphtha and ethane [1,2]. With the increasing consumption of petroleum resources, the production of calcium carbide from coal, acetylene from calcium carbide and water, and then hydrogenation to ethylene has emerged as a new alternative approach to produce ethylene, which is more economically feasible in areas rich in coal resources.…”

Section: Introductionmentioning

confidence: 99%

Pure Acetylene Semihydrogenation over Ni–Cu Bimetallic Catalysts: Effect of the Cu/Ni Ratio on Catalytic Performance

et al. 2020

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Ethylene is an important chemical raw material and with the increasing consumption of petroleum resources, the production of ethylene through the calcium carbide acetylene route has important research significance. In this work, a series of bimetallic catalysts with different Cu/Ni molar ratios are prepared by co-impregnation method for the hydrogenation of calcium carbide acetylene to ethylene. The introduction of an appropriate amount of Cu effectively inhibits not only the formation of ethane and green oil, thus increasing the selectivity of ethylene, but also the formation of carbon deposits, which improves the stability of the catalyst. The ethylene selectivity of the Ni–Cu bimetallic catalyst increases from 45% to 63% compared with the Ni monometallic counterpart and the acetylene conversion still can reach 100% at the optimal conditions of 250 °C, 8000 mL·g−1·h−1 and V(H2)/V(C2H2) = 3. X-ray diffraction and transmission electron microscopy confirmed that the metal particles were highly dispersed on the support, High-resolution transmission electron microscopy and H2-Temperature programmed reduction proved that there was an interaction between Ni and Cu, combined with X-ray photoelectron spectroscopy and density functional theory calculations results, Cu transferred electrons to Ni changed the Ni electron cloud density in NiCux catalysts, thus reducing the adsorption of acetylene and ethylene, which is favorable to ethylene selectivity.

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Section: Introductionmentioning

confidence: 99%

Pure Acetylene Semihydrogenation over Ni–Cu Bimetallic Catalysts: Effect of the Cu/Ni Ratio on Catalytic Performance

et al. 2020

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“…The high stability of Cu 2 (OH) 2 CO 3 (T140‐R150) might be associated with the low reaction temperature. It was reported that the core‐shell Pd@carbon nanoparticles supported on carbon nanotubes (Pd@C/CNTs) showed excellent stability in acetylene hydrogenation [61] . The formation of the porous carbon matrix in Cu 2 (OH) 2 CO 3 (T140‐R150) might pose steric hindrance to the chain growth of linear hydrocarbons, thus suppressing the undesired oligomerization and polymerization.…”

Section: Resultsmentioning

confidence: 99%

High‐Performance Catalysts Derived from Cupric Subcarbonate for Selective Hydrogenation of Acetylene in an Ethylene Stream

Zeng

Wang

et al. 2021

Eur J Inorg Chem

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A high‐performance base metal catalyst for acetylene selective hydrogenation was prepared from cupric subcarbonate (Cu2(OH)2CO3) by thermal treatment with an acetylene‐containing gas followed by hydrogen reduction. The characterization results revealed that the copper catalyst was composed of interstitial copper carbide (CuxC) and metal Cu, which were embedded in porous carbon matrix. The CuxC crystallites, which showed outstanding hydrogenation activity, were derived from the hydrogen reduction of copper (II) acetylide (CuC2) which was generated from the reaction between acetylene and Cu2(OH)2CO3. The Cu particles and porous carbon were generated from the unavoidable thermal decomposition of CuC2. The prepared Cu‐derived catalyst completely removed the acetylene impurity in an ethylene stream with a very low over‐hydrogenation selectivity at 110 °C and atmospheric pressure. No obvious deactivation was observed in a 180‐h test run. In the Cu‐derived catalyst, CuxC served as the catalytic site for H2 dissociation, Cu mainly functioned as the site for selective hydrogenation of acetylene, whereas the porous carbon matrix posed a steric hindrance effect on the chain growth of linear hydrocarbons so as to suppress the undesired oligomerization.

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“…This change is reversible in Figure S21, where the conversion of acetylene can be maintained when the reaction temperature is back to 190 °C, i.e., there are no severe catalyst deactivation. Therefore, the observed low activity in the higher temperature regime is ascribed to the trade‐off between the acetylene hydrogenation and its desorption with the temperature rather than the result of an irreversible deactivation of the catalysts …”

Section: Resultsmentioning

confidence: 99%

Adsorption Site Regulation to Guide Atomic Design of Ni–Ga Catalysts for Acetylene Semi‐Hydrogenation

Cao

Zhang

et al. 2020

Angewandte Chemie

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Atomic regulation of metal catalysts has emerged as an intriguing yet challenging strategy to boost product selectivity. Here, we report a density functional theory‐guided atomic design strategy for the fabrication of a NiGa intermetallic catalyst with completely isolated Ni sites to optimize acetylene semi‐hydrogenation processes. Such Ni sites show not only preferential acetylene π‐adsorption, but also enhanced ethylene desorption. The characteristics of the Ni sites are confirmed by multiple characterization techniques, including aberration‐corrected high‐resolution scanning transmission electron microscopy and X‐ray absorption spectrometry measurements. The superior performance is also confirmed experimentally against a Ni5Ga3 intermetallic catalyst with partially isolated Ni sites and against a Ni catalyst with multi‐atomic ensemble Ni sites. Accordingly, the NiGa intermetallic catalyst with the completely isolated Ni sites shows significantly enhanced selectivity to ethylene and suppressed coke formation.

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Pd@C core–shell nanoparticles on carbon nanotubes as highly stable and selective catalysts for hydrogenation of acetylene to ethylene

Cited by 38 publications

References 26 publications

Pure Acetylene Semihydrogenation over Ni–Cu Bimetallic Catalysts: Effect of the Cu/Ni Ratio on Catalytic Performance

Pure Acetylene Semihydrogenation over Ni–Cu Bimetallic Catalysts: Effect of the Cu/Ni Ratio on Catalytic Performance

High‐Performance Catalysts Derived from Cupric Subcarbonate for Selective Hydrogenation of Acetylene in an Ethylene Stream

Adsorption Site Regulation to Guide Atomic Design of Ni–Ga Catalysts for Acetylene Semi‐Hydrogenation

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