Quasi Pd1Ni single-atom surface alloy catalyst enables hydrogenation of nitriles to secondary amines

Wang, Hengwei; Luo, Qiquan; Liu, Wei; Lin, Yue; Guan, Qiaoqiao; Zheng, Xusheng; Pan, Haibin; Zhu, Junfa; Sun, Zhihu; Wei, Shiqiang; Yang, Jinlong; Lu, Junling

doi:10.1038/s41467-019-12993-x

Cited by 109 publications

(116 citation statements)

References 69 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%

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%

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

Wang

2020

Chin. J. Chem.

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“…[25][26][27] Currently, the difficulty in controlling the favorable interactions and synergistic effects in SAAs has limited their applications in electrocatalysis. [28][29][30][31][32][33][34] Intermetallics possess long-range atomic ordering and isolated metallic atoms on the surface, which could serve as a promising matrix to construct SAAs, yet that has not been explored.…”

Section: Introductionmentioning

confidence: 99%

A Tensile‐Strained Pt–Rh Single‐Atom Alloy Remarkably Boosts Ethanol Oxidation

et al. 2021

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which is also considered a biorenew able energy carrier. However, the anodic ethanol oxidation reaction (EOR) is a complicated and kinetically sluggish process, involving the transfer of multiple electrons and various reaction intermediates and products. Typically, the C2-pathway dominates the EOR in both acidic and alkaline electrolytes, resulting in the formation of acetic acid or acetate by delivering four electrons, and acetaldehyde by delivering two electrons, respectively. The C1-pathway, which involves complete oxidation and the transfer of 12 electrons generating CO 2 or carbonate, is preferred to the C2-pathway, aiming for maximum DEFCs efficiency. [1][2][3][4][5] Specially, highly efficient catalysts have been developed by engineering Pt-based nanocrystals, and the C1-pathway selectivity has been promoted by Rh-based catalysts. [6][7][8][9] In designing electrochemical surfaces toward maximum performance, modifying the electronic structure and strain of catalytic surfaces are considered state-of-the-art strategies, which can for instance be achieved by introducing metals with different intrinsic reactivities and constructing core-shell nanostructures, respectively. [10][11][12][13][14][15] Combining these approaches in a rational manner would be a promising way to substantially improve the EOR, yet the underlying knowledge about their contributions is largely lacking. [10][11][12][13][14][15][16][17][18] Therefore, it is highly desirable to employ tailored nanostructures to resolve these important issues and contribute to the practical deployment of DEFCs by identifying versatile EOR electrocatalysts possessing high atom utilization of noble metals, high mass-normalized activity at low overpotentials, high C1-pathway selectivity, long-term durability, and superior anti-poisoning ability. [1] To maximize atom utilization, single-atom catalysts (SACs) have emerged as one of the most promising frontiers in materials chemistry. [19][20][21] Using specific support materials such as reducible metal oxides, activated carbons, and anisotropic materials such as MoS 2 , single atoms of catalytically metals can be stabilized, which exhibit intriguing physicochemical properties compared with their counterpart clusters and nanoparticles. [22][23][24] Typically, high-performance EOR catalysts should facilitate multiple dehydrogenation and oxidation steps as well as CC bond cleavage reactions. All these reactions typically require ensembles of surface metal atoms, implying that thisThe rational design and control of electrocatalysts at single-atomic sites could enable unprecedented atomic utilization and catalytic properties, yet it remains challenging in multimetallic alloys. Herein, the first example of isolated Rh atoms on ordered PtBi nanoplates (PtBi-Rh 1 ) by atomic galvanic replacement, and their subsequent transformation into a tensile-strained Pt-Rh single-atom alloy (PtBi@PtRh 1 ) via electrochemical dealloying are presented. Benefiting from the Rh 1 -tailored Pt (110) surface with tensile strain, the PtBi@...

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“…The importance of strong metal-support interactions has long been recognized 5 . Of special interest is the stabilization of single-metal atoms on a support, which is rapidly becoming a new frontier in materials chemistry and catalysis [6][7][8][9][10][11] . The single-atom nature of the catalysts can overcome the scarcity of particular elements, such as precious group metals, ubiquitous in catalysis 1,8,12 .…”

Section: Introductionmentioning

confidence: 99%

Stability of heterogeneous single-atom catalysts: a scaling law mapping thermodynamics to kinetics

Zhang

Wang

et al. 2020

npj Comput Mater

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Heterogeneous single-atom catalysts (SACs) hold the promise of combining high catalytic performance with maximum utilization of often precious metals. We extend the current thermodynamic view of SAC stability in terms of the binding energy (Ebind) of single-metal atoms on a support to a kinetic (transport) one by considering the activation barrier for metal atom diffusion. A rapid computational screening approach allows predicting diffusion barriers for metal–support pairs based on Ebind of a metal atom to the support and the cohesive energy of the bulk metal (Ec). Metal–support combinations relevant to contemporary catalysis are explored by density functional theory. Assisted by machine-learning methods, we find that the diffusion activation barrier correlates with (Ebind)2/Ec in the physical descriptor space. This diffusion scaling-law provides a simple model for screening thermodynamics to kinetics of metal adatom on a support.

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Quasi Pd1Ni single-atom surface alloy catalyst enables hydrogenation of nitriles to secondary amines

Cited by 109 publications

References 69 publications

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

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

A Tensile‐Strained Pt–Rh Single‐Atom Alloy Remarkably Boosts Ethanol Oxidation

Stability of heterogeneous single-atom catalysts: a scaling law mapping thermodynamics to kinetics

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