scholarly journals Modulating the local coordination environment of single-atom catalysts for enhanced catalytic performance

Nano Research ◽  
2020 ◽  
Vol 13 (7) ◽  
pp. 1842-1855 ◽  
Author(s):  
Xinyuan Li ◽  
Hongpan Rong ◽  
Jiatao Zhang ◽  
Dingsheng Wang ◽  
Yadong Li
Keyword(s):  
Catalytic Performance ◽  
Single Atom ◽  
Coordination Environment ◽  
Local Coordination

scholarly journals Unraveling the coordination structure-performance relationship in Pt1/Fe2O3 single-atom catalyst

2019 ◽  
Vol 10 (1) ◽  
Author(s):  
Yujing Ren ◽  
Yan Tang ◽  
Leilei Zhang ◽  
Xiaoyan Liu ◽  
Lin Li ◽  
...  
Keyword(s):  
Coordination Chemistry ◽  
Homogeneous Catalysis ◽  
Catalytic Performance ◽  
Inert Atmosphere ◽  
Single Atom ◽  
Unique Role ◽  
Local Coordination ◽  
Single Atoms ◽  
Heterogeneous And Homogeneous Catalysis

Abstract Heterogeneous single-atom catalyst (SAC) opens a unique entry to establishing structure–performance relationship at the molecular level similar to that in homogeneous catalysis. The challenge lies in manipulating the coordination chemistry of single atoms without changing single-atom dispersion. Here, we develop an efficient synthetic method for SACs by using ethanediamine to chelate Pt cations and then removing the ethanediamine by a rapid thermal treatment (RTT) in inert atmosphere. The coordination chemistry of Pt single atoms on a Fe2O3 support is finely tuned by merely adjusting the RTT temperature. With the decrease in Pt-O coordination number, the oxidation state of Pt decreases, and consequently the hydrogenation activity increases to a record level without loss of chemoselectivity. The tunability of the local coordination chemistry, oxidation states of the metal, and the catalytic performance of single atoms reveals the unique role of SACs as a bridge between heterogeneous and homogeneous catalysis.

Revealing the Correlation between Catalytic Selectivity and the Local Coordination Environment of Pt Single Atom

Nano Letters ◽  
2020 ◽  
Vol 20 (9) ◽  
pp. 6865-6872
Author(s):  
Yong Xu ◽  
Mingyu Chu ◽  
Fangfang Liu ◽  
Xuchun Wang ◽  
Yu Liu ◽  
...  
Keyword(s):  
Single Atom ◽  
Coordination Environment ◽  
Local Coordination ◽  
Catalytic Selectivity

scholarly journals Regulating coordination number in atomically dispersed Pt species on defect-rich graphene for n-butane dehydrogenation reaction

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Xiaowen Chen ◽  
Mi Peng ◽  
Xiangbin Cai ◽  
Yunlei Chen ◽  
Zhimin Jia ◽  
...  
Keyword(s):  
Coordination Number ◽  
Density Functional ◽  
Activation Barrier ◽  
Density Functional Theory Calculation ◽  
Catalytic Performance ◽  
Atomic Level ◽  
Metal Nanoparticle ◽  
Single Atom ◽  
Nano Structure ◽  
Theory Calculation

AbstractMetal nanoparticle (NP), cluster and isolated metal atom (or single atom, SA) exhibit different catalytic performance in heterogeneous catalysis originating from their distinct nanostructures. To maximize atom efficiency and boost activity for catalysis, the construction of structure–performance relationship provides an effective way at the atomic level. Here, we successfully fabricate fully exposed Pt3 clusters on the defective nanodiamond@graphene (ND@G) by the assistance of atomically dispersed Sn promoters, and correlated the n-butane direct dehydrogenation (DDH) activity with the average coordination number (CN) of Pt-Pt bond in Pt NP, Pt3 cluster and Pt SA for fundamentally understanding structure (especially the sub-nano structure) effects on n-butane DDH reaction at the atomic level. The as-prepared fully exposed Pt3 cluster catalyst shows higher conversion (35.4%) and remarkable alkene selectivity (99.0%) for n-butane direct DDH reaction at 450 °C, compared to typical Pt NP and Pt SA catalysts supported on ND@G. Density functional theory calculation (DFT) reveal that the fully exposed Pt3 clusters possess favorable dehydrogenation activation barrier of n-butane and reasonable desorption barrier of butene in the DDH reaction.

Oxygen defects-stabilized heterogeneous single atom catalysts: preparation, property and catalytic application

2021 ◽  
Author(s):  
Lei Zhang ◽  
Xiu-Fei Zhao ◽  
Zhengqiu Yuan ◽  
Ming Wu ◽  
Hu Zhou
Keyword(s):  
Electronic Structure ◽  
Single Atom ◽  
Metal Species ◽  
Coordination Environment ◽  
Chemical Catalysis ◽  
Catalytic Application ◽  
Oxygen Defects ◽  
Catalysts Preparation

Single atom catalysts (SACs) show outstanding activity and selectivity in chemical catalysis owing to its unique electronic structure and unsaturated coordination environment, in which every dispersed metal species on support...

scholarly journals Highly dispersed Pt atoms and clusters on hydroxylated indium tin oxide: A view from first-principles calculations

2021 ◽  
Author(s):  
Simran Kumari ◽  
Philippe Sautet
Keyword(s):  
Heterogeneous Catalysis ◽  
Metal Atom ◽  
Tin Oxide ◽  
Indium Tin Oxide ◽  
First Principles ◽  
Catalytic Performance ◽  
Small Cluster ◽  
Single Atom ◽  
First Principles Calculations ◽  
Highly Dispersed

Supported single-atom and small cluster catalysts have become highly popular in heterogeneous catalysis. These catalysts can maximize the metal atom utilization while still showcasing superior catalytic performance. One of the...

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

2020 ◽  
Vol 6 (1) ◽  
Author(s):  
Ya-Qiong Su ◽  
Long Zhang ◽  
Yifan Wang ◽  
Jin-Xun Liu ◽  
Valery Muravev ◽  
...  
Keyword(s):  
Metal Atom ◽  
Density Functional ◽  
Activation Barrier ◽  
Scaling Law ◽  
Precious Metals ◽  
Catalytic Performance ◽  
Single Atom ◽  
Atom Diffusion ◽  
Computational Screening ◽  
Metal Support

Abstract 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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