Evaluating the Stability of Single-Atom Catalysts with High Chemical Activity

Wang, Chen Santillan; Wang, Hui; Wu, Ruqian; Ragan, Regina

doi:10.1021/acs.jpcc.8b06621

Cited by 22 publications

(18 citation statements)

References 78 publications

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“…The CO oxidation performance of SACs could also be largely affected by the local geometric structure of single atom centers. For instance, Wang et al employed DFT calculations to identify how the local molecular environment on graphene can be used to stabilize and tune the electronic structure of single Pt atoms for high CO oxidation efficiency . Results indicate that the Pt–C interaction at the vacancy defects in graphene is critical for the stabilization of single Pt atoms, which facilitates the charge transfer between Pt and O 2 and results in the enhanced CO oxidation activity.…”

Section: Applicationsmentioning

confidence: 99%

Supported Noble‐Metal Single Atoms for Heterogeneous Catalysis

et al. 2019

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metal atoms are highly desirable for supported noble-metal (NM) catalysts. [2] Single-atom catalyst (SAC), defined as a catalyst composing only isolated singleatom active sites on supports, was first introduced by Zhang and co-workers in 2011. [3] Owing to the single-atom feature of active sites, SACs provide great advantages in minimizing the usage of precious metal with a 100% atom-utilization efficiency, which thus result in an improved catalytic reactivity, and have aroused extensive attention in the field of catalysis over the past few years. [4] Meanwhile, since the electronic properties of active sites greatly depend on the size and shape of metal particles, which then governs the performance of a catalyst, [5] downsizing metal nanoparticles (NPs) to single atom with the decreased low coordination and the quantized orbital of active sites, is recognized as the other important factor in tuning the catalytic performance of SACs. [5,6] However, due to the tendency of aggregation of single atoms during preactivation and under reaction procedures, utilization of metal/support interactions to immobilize single atom on supports plays a crucial role on the stability of SACs, and the development of effective synthesis strategies is indispensable to realize the distribution and chemical bonding of active sites on supports for the further applications of SACs.In particular, high density of active sites with well-defined local coordination structure to give appreciable catalytic activity/ selectivity and long-term stability are the ultimate goals in catalysis. [7] Thus, long-standing interest exists in fabricating heterogeneous catalysts that feature atomically dispersed metal atoms as active sites for catalytic processes. Even though, considerable efforts have been devoted to, and many advances have been achieved in supported NM-SACs for various heterogeneous catalytic applications, inclusive of CO oxidation, selective hydrogenation, water-gas shift, CO 2 reduction, electrocatalysis, and etc. [2b,7b,8] The achievements from recent studies have greatly contributed to the fast development of single-atom catalysis and paves the way for the rational design of efficient SACs in much broader catalytic systems.In this review, we will focus on this new kind of material, with great attention on the geometric and electronic structure of the single atom active sites, as well as its stability on supports. The recently developed strategies for synthesizing SACs with high metal loading and precise structure are also Single-atom catalysts (SACs), with atomically distributed active metal sites on supports, serve as a newly advanced material in catalysis, and open broad prospects for a wide variety of catalytic processes owing to their unique catalytic behaviors. To construct SACs with precise structures and high density of accessible single-atom sites, while preventing aggregation to large nanoparticles, various strategies for their chemical synthesis have been recently developed by improving the distribution and chemical bondi...

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Section: Applicationsmentioning

confidence: 99%

Supported Noble‐Metal Single Atoms for Heterogeneous Catalysis

et al. 2019

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“…In addition, more recent HAADF-STEM measurements have even observed single Pt atoms dispersed on undoped [15,16] and nitrogendoped [17] graphene, which show high catalytic activities and CO tolerance. Theoretically, on the other hand, firstprinciples calculations based on density functional theory (DFT) have been performed extensively to clarify the properties of graphene-supported Pt clusters from viewpoints of geometric [18][19][20][21][22][23][24][25][26][27][28][29][30][31][32][33][34] and magnetic [35][36][37][38][39][40][41][42][43][44] structures, molecular adsorptions [45][46][47][48][49][50], CO tolerance [51][52][53][54], and catalytic reactions such as CO oxidation [55][56][57][58][59][60], decomposition of O 3…”

Section: Introductionmentioning

confidence: 99%

Enhanced CO tolerance of Pt clusters supported on graphene with lattice vacancies

et al. 2020

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The adsorption of CO on Pt 4 clusters supported on graphene with lattice vacancies is studied theoretically using the first-principles calculation. Our results show that the electronic structure of the graphene-supported Pt 4 clusters is significantly modified by the interaction with carbon dangling bonds. As a result the adsorption energy of CO at a Pt site decreases almost linearly with the lowering of the Pt d-band center, in analogy with the linear law previously reported for CO adsorption on various Pt surfaces. An exceptional behavior is found for Pt 4 supported on graphene with a tetravacancy, where CO adsorption is noticeably weaker than predicted by the shift in the d-band center. Detailed electronic structure analyses reveal that the deviation from the linear scaling can be attributed to lack of Pt d states near the Fermi level that hybridize with CO molecular orbitals. The weakening of CO adsorption on the Pt 4 clusters is considered as a manifestation of the support effect of graphene, and leads to the enhancement of CO poisoning tolerance that is crucial for developing high-performance Pt cluster catalysts.

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“…The catalytic activity mostly depends on a number of active sites and their accessibilities. Catalytic activity can be tuned by manipulating the nanoparticles sizes or by producing shaped nanoparticles with exposed facets [2][3][4][5]. Keys factors for catalytic properties are not very well known and atoms with the different environments are mostly showed different catalytic activity.…”

Section: Introductionmentioning

confidence: 99%

“…Singlemetal atom catalysts (SMACs) have shown better activity compared with subnanometer nanoparticles materials. As limited by the change in morphologies of nanoparticles, a concept of SMACs has emerged because it only way remaining to maximize efficiency of catalyst [4,5]. Many single Co atoms homogeneous catalysts have been reported (Figure 1a, b) [7], in which single metal atom is supported by the bulky organic functional groups; their activity and accessibility depends on the organic environment around the single metal atom.…”

Section: Introductionmentioning

confidence: 99%

“…The preparation of stable SMACs is still challenging because high energy of a single atom leads to agglomeration and makes them unstable under reaction conditions at the industrial level. An effective way for a synthesis of SMACs via increasing the interaction between a metal atom and support [4]. In general process, by reducing the size of nanocatalyst and bring them at atomic scale, we are trying to heterogenize homogeneous catalysts on heterogeneous supports.…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Cobalt Single Atom Heterogeneous Catalyst: Method of Preparation, Characterization, Catalysis, and Mechanism

Singh¹,

Kumar²,

Singh³

2019

Cobalt Compounds and Applications

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Transition metal nanoparticles and metal oxide have been used extensively for a wide range of applications in electrochemical reactions (HER, ORR, OER) and energy storage (supercapacitors batteries). To make less expensive, the use of transition metal at minimum metal contents without compromising the catalytic activity could be one way. Most of the catalytic process takes place on the surface and reaction dynamic can be manipulated by changing the particle size and shape. For a long time, single metal atom organometallic compounds have been used as a catalyst at the industrial level. However, problems with the homogeneous catalyst to recover back at the end of the process lead to development of heterogeneous single-atom catalysts with equal activity like a homogeneous catalyst. Cobalt single atom has received a tremendous interest of the scientific community due to its excellent catalytic activity and recyclability. Cobalt single-atom catalyst has shown better performance compared with sub-nanometer nanoparticles catalyst for ORR, OER, and HER. This chapter is conferring method of preparation of carbon-based single Co atoms heterogeneous catalyst, their application for ORR, OER, HER reactions, and mechanistic investigations through DFT calculations. The role of single Co metal atoms and anchoring using N or heteroatoms is discussed and compared.

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Evaluating the Stability of Single-Atom Catalysts with High Chemical Activity

Cited by 22 publications

References 78 publications

Supported Noble‐Metal Single Atoms for Heterogeneous Catalysis

Supported Noble‐Metal Single Atoms for Heterogeneous Catalysis

Enhanced CO tolerance of Pt clusters supported on graphene with lattice vacancies

Cobalt Single Atom Heterogeneous Catalyst: Method of Preparation, Characterization, Catalysis, and Mechanism

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