Structural and Kinetics Understanding of Support Effects in Pd-Catalyzed Semi-Hydrogenation of Acetylene

Cao, Yueqiang; Ge, Xiaohu; Li, Yurou; Si, Rui; Sui, Zhi‐Jun; Zhou, Jinghong; Duan, Xuezhi

doi:10.1016/j.eng.2020.06.023

Cited by 41 publications

(30 citation statements)

References 53 publications

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“…7a , the C 2 H 2 -TPD profile of the Ni catalyst presents three legible peaks centered at 168, 320, and 457 °C. According to previous studies, the peak at the temperature of 168 °C is attributed to the desorption of weakly π-adsorbed C 2 H 2 , and the peaks located at 320 and 457 °C are corresponded to the desorption of C 2 H 2 species and/or the corresponding C 2 -fragments formed at the elevated temperature di-σ-bonded on bridge Ni sites and multi-σ-bonded on hollow Ni sites, respectively 42 – 44 . The C 2 H 2 -TPD profile of the NiSb catalyst shows two visible desorption peaks located at 124 and 286 °C corresponded to π-adsorbed and σ-adsorbed C 2 H 2 , respectively, which are lower than those of the peaks seen with the profile of the Ni catalyst.…”

Section: Resultsmentioning

confidence: 76%

Mechanism driven design of trimer Ni1Sb2 site delivering superior hydrogenation selectivity to ethylene

Dou

Cao

et al. 2022

Nat Commun

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Mechanism driven catalyst design with atomically uniform ensemble sites is an important yet challenging issue in heterogeneous catalysis associated with breaking the activity-selectivity trade-off. Herein, a trimer Ni1Sb2 site in NiSb intermetallic featuring superior selectivity is elaborated for acetylene semi-hydrogenation via a theoretical guidance with a precise synthesis strategy. The trimer Ni1Sb2 site in NiSb intermetallic is predicted to endow acetylene reactant with an adequately but not excessively strong σ-adsorption mode while ethylene product with a weak π-adsorption one, where such compromise delivers higher ethylene formation rate. An in-situ trapping of molten Sb by Ni strategy is developed to realize the construction of Ni1Sb2 site in the intermetallic P63/mmc NiSb catalysts. Such catalyst exhibits ethylene selectivity up to 93.2% at 100% of acetylene conversion, significantly prevailing over the referred Ni catalyst. These insights shed new lights on rational catalyst design by taming active sites to energetically match targeted reaction pathway.

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Section: Resultsmentioning

confidence: 76%

Mechanism driven design of trimer Ni1Sb2 site delivering superior hydrogenation selectivity to ethylene

Dou

Cao

et al. 2022

Nat Commun

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“…Unfortunately, these properties are closely linked to each other and generally do not allow simultaneous optimization . From a structural perspective, most efforts devoted to optimizing Pd catalysts are focused on the geometric (Pd–Pd coordination) and electronic (d-band center) structures of Pd sites. − Typical strategies include blocking active Pd sites by additives − and isolating Pd atoms in support structures ,− or intermetallic structures , (e.g., PdAg, , PdGa, − PdIn, , and PdZn). Despite the significant progress that has been achieved in recent years, developing catalysts with extremely wide operating windows for safe and stable operation in front-end processes remains a great challenge.…”

Section: Introductionmentioning

confidence: 99%

Highly Selective Acetylene Semihydrogenation Catalyst with an Operation Window Exceeding 150 °C

et al. 2021

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The operating window (OW) is a primary performance criterion for the selective hydrogenation of acetylene in excess ethylene. Currently, most state-of-the-art catalyst systems have an OW of less than 50 °C in front-end processes. Selective acetylene hydrogenation catalysts with an OW wider than 100 °C are rare. Here, we demonstrate a facile stepwise chemical method to synthesize calcite-supported PdBi intermetallic compounds (PdBi/Calcite) that feature isolated and electron-rich Pd atoms as active sites for acetylene hydrogenation. Beneficial from the extremely weak ethylene absorption abilities and the stable structures against the formation of β-PdH x , PdBi/Calcite exhibit >99% selectivity to C 2 H 4 in the whole temperature range tested (50−300 °C) and ∼100% C 2 H 2 conversion from 150 to 300 °C. As a result, an operation window exceeding 150 °C has been achieved.

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“…Noble‐metal catalysts ( e.g ., Pt, RuO 2 and IrO 2 ) demonstrate superior performance in HER or OER, but the natures of high‐cost and scarce resource inhibit their large‐scale applications [13–16] . Nevertheless, Ru is the cheapest among all the Pt‐group metals with about 2/3 price of Pt, and Ru‐based electrocatalysts exhibit outstanding activity for the alkaline water splitting [16–18] .…”

Section: Introductionmentioning

confidence: 99%

Constructing RuCoO_x/NC Nanosheets with Low Crystallinity within ZIF‐9 as Bifunctional Catalysts for Highly Efficient Overall Water Splitting

Tuo

Liu

Chen

et al. 2021

Chemistry An Asian Journal

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Electrocatalysts play a pivotal role in accelerating the sluggish electrochemical water splitting reaction. Herein, a Ru−Co oxides and carbon nitrides hybrid (RuCoOx/NC) electrocatalyst was constructed by employing ZIF‐9 to disperse Ru precursor and deliberately regulating the calcination temperature. The moderate calcination temperature results in the RuCoOx nanocomposites with small particle size and low crystallinity as well as the co‐existence of multi‐valence metal compounds, thus boosting the amount and species of active sites. Moreover, the strong interactions between Co and Ru species induce the electron transfer from Co to Ru, thus enhancing the adsorption of anion intermediates on the electron‐deficient Co species and the proton capturing capacity of electron‐sufficient Ru species. As a result, the optimized RuCoOx/NC‐350 catalyst behaved good electrocatalytic activities with 73 and 210 mV overpotential to achieve 10 mA cm−2 for HER and OER, respectively. Remarkably, it showed good durability by holding at 100 mA cm−2 for 100 h in HER and 50 mA cm−2 for 24 h in OER with small activity decline. This study may shed new light on the rational construction of highly efficient Ru‐based catalysts for electrochemical water splitting.

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Structural and Kinetics Understanding of Support Effects in Pd-Catalyzed Semi-Hydrogenation of Acetylene

Cited by 41 publications

References 53 publications

Mechanism driven design of trimer Ni1Sb2 site delivering superior hydrogenation selectivity to ethylene

Mechanism driven design of trimer Ni1Sb2 site delivering superior hydrogenation selectivity to ethylene

Highly Selective Acetylene Semihydrogenation Catalyst with an Operation Window Exceeding 150 °C

Constructing RuCoO_x/NC Nanosheets with Low Crystallinity within ZIF‐9 as Bifunctional Catalysts for Highly Efficient Overall Water Splitting

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Structural and Kinetics Understanding of Support Effects in Pd-Catalyzed Semi-Hydrogenation of Acetylene

Cited by 41 publications

References 53 publications

Mechanism driven design of trimer Ni1Sb2 site delivering superior hydrogenation selectivity to ethylene

Mechanism driven design of trimer Ni1Sb2 site delivering superior hydrogenation selectivity to ethylene

Highly Selective Acetylene Semihydrogenation Catalyst with an Operation Window Exceeding 150 °C

Constructing RuCoOx/NC Nanosheets with Low Crystallinity within ZIF‐9 as Bifunctional Catalysts for Highly Efficient Overall Water Splitting

Contact Info

Product

Resources

About

Constructing RuCoO_x/NC Nanosheets with Low Crystallinity within ZIF‐9 as Bifunctional Catalysts for Highly Efficient Overall Water Splitting