Pt-O4 moiety induced electron localization toward In2O-Triggered acetylene Semi-Hydrogenation

Li, Yurou; Cao, Yueqiang; Ge, Xiaohu; Zhang, Hao; Yan, Kelin; Zhang, Jing; Qia, Gang; Jiang, Zheng; Gong, X. G.; Li, Aoming; Zhou, Xin; Wang, Yuan; Duan, Xuezhi

doi:10.1016/j.jcat.2022.02.005

Cited by 13 publications

(14 citation statements)

References 53 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Through reasonable data extraction, feature engineering and logical reasoning, it is possible to extract the key influencing factors from complex electronic structure information. , Another easily overlooked situation is the indirect electronic modulation by noble metals. For example, reducible metal oxides can be richer in electrons when loaded noble metal atoms are exposed in a hydrogen atmosphere. , The reason lies in that noble-metal species enhance the hydrogen dissociation activity and increase content of oxygen vacancies on the surface of the support accordingly. The increased oxygen vacancies as active sites again enhanced the catalytic performance such as the selective semihydrogenation of acetylene.…”

Section: The Geometric and Electronic Effects For Selective Hydrogena...mentioning

confidence: 99%

“…For example, reducible metal oxides can be richer in electrons when loaded noble metal atoms are exposed in a hydrogen atmosphere. 396,397 The reason lies in that noblemetal species enhance the hydrogen dissociation activity and increase content of oxygen vacancies on the surface of the support accordingly. The increased oxygen vacancies as active sites again enhanced the catalytic performance such as the selective semihydrogenation of acetylene.…”

Section: Acs Catalysis Pubsacsorg/acscatalysismentioning

confidence: 99%

See 1 more Smart Citation

Geometric and Electronic Effects in Hydrogenation Reactions

et al. 2022

View full text Add to dashboard Cite

Selective hydrogenation has a long history of being an important reaction process for the preparation of high-value chemicals. The geometric and electronic structures of the catalysts largely determine their basic catalytic performance, including activity, selectivity, and stability. However, the complexity of the components and structures of the catalytic active sites poses a significant challenge to the characterization and the sequential performance attribution. On the basis of summarizing the geometric and electronic structure research in this field, this Review will pay special attention to the adsorption and activation modes of reactants, reaction kinetics, identification and classification of structural sensitivity, methods for geometric and electronic regulation, and distinctive concepts for catalyst design, to enlighten the further development of high-efficiency hydrogenation catalysts.

show abstract

Section: The Geometric and Electronic Effects For Selective Hydrogena...mentioning

confidence: 99%

Section: Acs Catalysis Pubsacsorg/acscatalysismentioning

confidence: 99%

Geometric and Electronic Effects in Hydrogenation Reactions

et al. 2022

View full text Add to dashboard Cite

show abstract

“…Upon creating the oxygen vacancies, the surrounding In and O sites form the In 3 O 5 ensemble sites, schematically shown in Figure a, which were proven to be stable and active for acetylene semihydrogenation to ethylene. To further improve the performance of indium oxide catalysts, especially the hydrogenation activity, our group recently reported a theoretical-guided atomic design strategy with experimental verification to fabricate an Pt-O 4 -In 2 O ensemble sites for acetylene semihydrogenation (Figure b) . Introducing single-atom Pt into the indium oxides to create a Pt–O 4 moiety was found to significantly increase the electron localization within the moiety and thus enhance the frustrated In–O Lewis pairs within the In 2 O site (Figure d,e).…”

Section: Atomic-level Regulation For Active Sitesmentioning

confidence: 99%

Section: Atomic-level Regulation For Active Sitesmentioning

confidence: 99%

“…To further improve the performance of indium oxide catalysts, especially the hydrogenation activity, our group recently reported a theoretical-guided atomic design strategy with experimental verification to fabricate an Pt-O 4 -In 2 O ensemble sites for acetylene semihydrogenation (Figure 15b). 147 Introducing single-atom Pt into the indium oxides to create a Pt−O 4 moiety was found to significantly increase the electron localization within the moiety and thus enhance the frustrated In−O Lewis pairs within the In 2 O site (Figure 15d,e). These unique electronic structures of the ensemble sites were further demonstrated to promote the hydrogen activation via the heterolytic dissociation of hydrogen, as evidenced by the decreased energy barrier (Figure 15c) and Bader charge analysis for the corresponding transition state (Figure 15f,g).…”

Section: Oxygen Vacancy and Interfacialmentioning

confidence: 99%

See 1 more Smart Citation

Mechanistic and Atomic-Level Insights into Semihydrogenation Catalysis to Light Olefins

Yan

Cao

et al. 2022

ACS Catal.

Self Cite

View full text Add to dashboard Cite

Semihydrogenations of alkynes and alkadienes to light olefins catalyzed by a heterogeneous catalyst are widely applied in the chemical industry, but it remains challenging to design high-performance catalysts for these processes. The well-developed synthesis methodologies, characterization techniques for catalyst structures, and theoretical calculations in recent decades render opportunities for understanding mechanisms and elaborating the structures of active sites at the atomic level. This Review summarizes recent advances in the mechanistic and atomic-level insights into semihydrogenation catalysis for alkynes and alkadienes to light olefins. The structure-sensitivity, information on active sites, and reaction kinetics are initially discussed to demonstrate the knowledge on the mechanistic and kinetics details of the hydrogenations of alkynes and alkadienes. We then introduce the regulations for the active sites, especially at the atomic level, based on three categories, i.e., site-isolation, local environment regulation, and oxygen vacancy and interfacial sites. Followed by the discussion on the conventional thermocatalytic hydrogenations, the emerging photocatalytic and electrocatalytic semihydrogenations of alkynes and alkadienes are further covered. Finally, we provide a brief overview on the current status of this field and a perspective for future study on the atomic-level design and regulation of catalysts for controlling the selectivity to target products.

show abstract

Dual effect of TiO₂ vacancy on Pd catalyst in acetylene hydrogenation: Boosting performance and capturing reaction heat

Yang

Shi

et al. 2023

AIChE Journal

View full text Add to dashboard Cite

Selective acetylene hydrogenation is a strongly exothermic process, easy to cause coking and metal agglomeration, and thus leads to deactivation. In this work, Pd/TiO 2 with different oxygen vacancies (V o ) were synthesized by controlling reduction temperature in 300-700 C, in which Pd/TiO 2 -HT300 (HT is reduction temperature) possessed the highest V o content. It was found highly dispersed Pd nanoparticles adjacent to more V o exhibited enhanced catalytic behavior (near 100% conversion at 55 C with 80% selectivity and turnover frequency of 0.12 s À1 ) due to hydrogen spillover generation and electron donation originating from V o sites, confirmed by in situ x-ray photoelectron spectroscopy, in situ Raman, and H 2 -temperature programmed desorption. More importantly, the increasing V o sites trap the released heat and devote to a decrease of heat accumulation over a single active Pd site, and consequently inhibit Pd agglomeration and polymerization, affirmed by high-resolution transmission electron microscopy, CO chemisorption, and thermogravimetric analysis.

show abstract

Pt-O4 moiety induced electron localization toward In2O-Triggered acetylene Semi-Hydrogenation

Cited by 13 publications

References 53 publications

Geometric and Electronic Effects in Hydrogenation Reactions

Geometric and Electronic Effects in Hydrogenation Reactions

Mechanistic and Atomic-Level Insights into Semihydrogenation Catalysis to Light Olefins

Dual effect of TiO₂ vacancy on Pd catalyst in acetylene hydrogenation: Boosting performance and capturing reaction heat

Contact Info

Product

Resources

About

Pt-O4 moiety induced electron localization toward In2O-Triggered acetylene Semi-Hydrogenation

Cited by 13 publications

References 53 publications

Geometric and Electronic Effects in Hydrogenation Reactions

Geometric and Electronic Effects in Hydrogenation Reactions

Mechanistic and Atomic-Level Insights into Semihydrogenation Catalysis to Light Olefins

Dual effect of TiO2 vacancy on Pd catalyst in acetylene hydrogenation: Boosting performance and capturing reaction heat

Contact Info

Product

Resources

About

Dual effect of TiO₂ vacancy on Pd catalyst in acetylene hydrogenation: Boosting performance and capturing reaction heat