Anchoring Cu1 species over nanodiamond-graphene for semi-hydrogenation of acetylene

Huang, Fei; Deng, Yuchen; Chen, Yunlei; Cai, Xiangbin; Peng, Mi; Jia, Zhimin; Xie, Jinglin; Xiao, Dequan; Wen, Xiaodong; Wang, Ning; Jiang, Zheng; Li, Hongyang; Ma, Ding

doi:10.1038/s41467-019-12460-7

Cited by 264 publications

(232 citation statements)

References 41 publications

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“…[ 226‐228 ] Tremendous efforts have been devoted to developing the methods of precise synthesis and to understanding the structure‐activity relations in a number of catalytic reactions. [ 226‐233 ] A thorough study of the particle size effect as well as taking the counterparts of ultrafine clusters and single atoms into account is highly necessary, which could provide a much deeper insight of structure‐activity relations and facilitate rational design of advanced metal catalysts. However, such studies in the real catalyst systems have been rarely reported.…”

Section: Particle Size Effect In Metal Catalysismentioning

confidence: 99%

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A Review on Particle Size Effect in Metal‐Catalyzed Heterogeneous Reactions

Wang

2020

Chin. J. Chem.

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Size of metal nanoparticles (NPs) plays decisive roles in metal-catalyzed heterogeneous reactions, due to the drastic variation of the geometric and electronic properties of metal NPs with size. Along with the development of controlled catalyst synthesis, tremendous efforts have been devoted to understanding the nature of the particle size effect. In particular, identification of the individual roles of size-dependent geometric and electronic effects on metal-catalyzed reactions is essential, but remains challenging since they are tightly hybridized together with particle size variation. In this review, we first discuss the fundamentals of the size-dependent geometric and electronic properties of metal NPs and their crucial roles in catalysis in general. Then we summarize the previous representative studies of the particle size effect, metal-by-metal, in heterogeneous catalysis. We highlighted the extension of particle size effect to ultrafine cluster and single-atom catalysts, the new frontiers in heterogeneous catalysis. In the followings, we further introduce the recent advances in disentangling the size-dependent geometric and electronic effects and unveiling their individual contributions to catalysis. Finally, we discuss the challenges and perspectives of investigations on the size effect in metal catalysis for the future studies. Mr. Hengwei Wang (left) received his B.Sc. degree from School of Chemistry and Materials Science, University of Science and Technology of China (USTC) in 2015. Then he Joined Professor Junling Lu's research group at USTC to pursue his doctorate in Physical Chemistry. His research focuses on atomically-precise design and synthesis of metal nanocatalysts for heterogeneous catalysis and unravelling their structure-reactivity relations at atomic scale. Prof. Junling Lu (right) received his Ph.D. degree from Institute of Physics, Chinese Academy of Sciences under the supervision of Prof. Hong-Jun Gao in 2007. During his Ph.D. studies, he visited Prof. Hans-Joachim Freund's group at Chemical Physics Department, Fritz-Haber-Institute, Max Planck Society as an exchange student in 2004-2006. After graduation, he spent three years in Prof. Peter C Stair's group at Northwestern University and then about two and a half years in Dr. Jeffrey W. Elam's group at Argonne National Laboratory as a Postdoc. In March 2013, he joined USTC as a Professor. His current research interest is atomically-precise design of a new generation of advanced catalysts through a combined wet-chemistry and atomic layer deposition (ALD) approach.

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Section: Particle Size Effect In Metal Catalysismentioning

confidence: 99%

“…Such impressive capability of coking inhibition is attributed to spatial confinement of single sites, which was also observed on other SACs. [ 233,237 ]…”

Section: Particle Size Effect In Metal Catalysismentioning

confidence: 99%

A Review on Particle Size Effect in Metal‐Catalyzed Heterogeneous Reactions

Wang

2020

Chin. J. Chem.

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“…[33][34][35] With the blooming development of SACs, the intrinsic defects have regarded as potential anchoring sites for stabilizing the metal species. [18,[36][37][38][39] Zhang and coworkers employed a pulsed laser deposition (PLD) technique to dig the desired vacancies with different sizes in the graphene matrix, and followed by metal dopant deposition. [36] To be investigated by aberration-corrected high-resolution transmission electron microscope (HRTEM), it shows that bi-vacancy or larger vacancies are the ideal trapping site for transition metal atoms, which have much larger atomic radii than carbon (Figure 2a,b).…”

Section: Defects Engineeringmentioning

confidence: 99%

“…[18] Besides, the defects of carbon supports are also critical for manipulating the electronic structure of SACs to increase the chemoselectivity relative to their bulk counterparts. [38,[40][41][42] For example, Ma and co-workers found that the catalyst with single Pd atoms on a defective nanodiamond-graphene support (Pd 1 / ND@G) shows an excellent performance for selective hydrogenation of acetylene to ethylene, in which the yield of ethylene is more than 90% under the 100% conversion efficiency of acetylene, and overwhelms that of Pd nanoclusters (Figure 2h). [41] The combination of XAFS and DFT analyses disclose that the atomic Pd is formed a pyramidal structure through bonding with three carbon atoms, which energetically favors desorption of the C 2 H 4 intermediate to suppress the further hydrogenation of the targeted product.…”

Section: Wwwadvancedsciencenewscommentioning

confidence: 99%

Structural Regulation and Support Coupling Effect of Single‐Atom Catalysts for Heterogeneous Catalysis

Liu

Ding

et al. 2020

Advanced Energy Materials

210

141

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Single atom catalysts (SACs) that integrate the merits of homogeneous and heterogeneous catalysts have been attracting considerable attention in recent years. The individual metal atoms of SACs can be stabilized on supports through various unsaturated chemical sites or space confinement for achieving the maximized atom utilization efficiency. Aside from the development of strategies for preparing high loading and high purity SACs, another key challenge in this field is precisely manipulating the geometric and electronic structure of catalytically active single metal sites, thus rendering the catalysts exceptionally reactive, selective, and stabile compared to their bulk counterparts. This review summarizes recent advancements in SACs for heterogeneous catalysis from the perspective of local structural regulation and the synergistic coupling effect between metal species and supports. Special emphasis is placed on the elucidation of the catalytic structure‐performance relationship in terms of coordination environment, valence state and metal‐support interactions by advanced characterization and theoretical studies. Select in situ or operando characterization techniques for tracking the SACs’ structure evolution under realistic conditions are highlighted. Finally, the challenges and opportunities are discussed to offer insight into the rational design of more intriguing SACs with high activity and distinct chemoselectivity.

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“…The alkyne semihydrogenation activity of single-atom Au was dependent on the substrates: structure insensitive for alkynols with γ-OH and unfunctionalized alkynes, while sensitive for alkynols with α-OH [47]. More recently, Ma and co-workers [48] reported that non-noble metal SACs Cu supported on nanodiamond-graphene exhibited 95% acetylene conversion and 98% ethylene selectivity.…”

Section: Introductionmentioning

confidence: 99%

Single-atom Pd dispersed on nanoscale anatase TiO2 for the selective hydrogenation of phenylacetylene

et al. 2020

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Combining the advantages of both heterogeneous and homogeneous catalysts, single-atom catalysts (SACs) with unique electronic properties have shown excellent catalytic properties. Herein, we report single-atom Pd dispersed on nanoscale TiO 2 prepared by self-assembly method as efficient and selective catalysts for the hydrogenation of phenylacetylene to styrene. The catalysts were characterized by N 2 adsorption/desorption, X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and X-ray absorption spectroscopy (XAS). 0.2Pd-TiO 2 (150°C) possessing dominant single-atom Pd species, exhibited a turnover frequency (TOF) of over 8000 h −1 with 91% selectivity towards styrene at room temperature. Further increasing Pd loading from 0.2% to 0.5% and 1.5% resulted in the decrease of activity probably due to the formation of Pd nanoparticles. Besides, the 0.2Pd-TiO 2 prepared by self-assembly strategy showed better catalytic performance than commercial 10%Pd/C and 0.2Pd-TiO 2 synthesized by using impregnation method.

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Anchoring Cu1 species over nanodiamond-graphene for semi-hydrogenation of acetylene

Cited by 264 publications

References 41 publications

A Review on Particle Size Effect in Metal‐Catalyzed Heterogeneous Reactions

A Review on Particle Size Effect in Metal‐Catalyzed Heterogeneous Reactions

Structural Regulation and Support Coupling Effect of Single‐Atom Catalysts for Heterogeneous Catalysis

Single-atom Pd dispersed on nanoscale anatase TiO2 for the selective hydrogenation of phenylacetylene

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