Reversible and cooperative photoactivation of single-atom Cu/TiO2 photocatalysts

Lee, Byoung‐Hoon; Park, Sunghak; Kim, Minho; Sinha, Arun K.; Lee, Seong Chan; Jung, Euiyeon; Chang, Woo Je; Lee, Kug‐Seung; Kim, Jeong Hyun; Cho, Sung‐Pyo; Kim, Hyungjun; Nam, Ki Tae; Hyeon, Taeghwan

doi:10.1038/s41563-019-0344-1

Cited by 529 publications

(408 citation statements)

References 46 publications

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“…[1] However, it is important to clarify that not all single-atom metal sites, especially non-exposed sites, can be referred to as active sites with contribution to catalysis, rendering the waste of inaccessible metals to a large degree. [2] For instance, it is found that metal sites near the external surface of catalysts are better able to catalyze the oxygen reduction reaction (ORR), an important reaction in metal-air batteries and fuel cells, whereas those buried in dense carbon matrix are inactive. [3] The low utilization of metal sites gives insufficient performance due to the poor mass transport through catalyst layers.…”

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confidence: 99%

Single‐Atom Iron Catalysts on Overhang‐Eave Carbon Cages for High‐Performance Oxygen Reduction Reaction

et al. 2020

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confidence: 99%

Single‐Atom Iron Catalysts on Overhang‐Eave Carbon Cages for High‐Performance Oxygen Reduction Reaction

et al. 2020

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“…Recently, along with the rapid development of SACs in the fields described above, SACs have shown distinctive performances and advantages in many other heterogeneous catalytic applications including photocatalysis, environmental remediation,41d,96 methanol steam reforming,33e and etc. However, the reaction rate per overall catalyst mass of SACs in most cases is still much lower than that of supported nanoparticle (NP)‐based catalysts, due to the lower loading of active atoms for the former.…”

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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“…Single-atom (SA) catalysts contain isolated single-metal atoms dispersed on a support surface, and represent the ultimate limit of atom use efficiency for catalysis 1,2 . Other desirable catalytic properties of SA catalysts include high selectivity, tunable high activity, and unique metal coordination environments [3][4][5][6] . As a result, SA catalysts have attracted tremendous attention as a new frontier in heterogeneous catalysis for many reactions, including oxidation 7,8 , hydrogenation 9,10 , electrocatalysis [11][12][13][14] , and so on 15,16 .…”

Section: Introductionmentioning

confidence: 99%

Stabilizing mechanism of single-atom catalysts on a defective carbon surface

et al. 2020

npj Comput Mater

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Single-atom (SA) catalysts represent the ultimate limit of atom use efficiency for catalysis. Promising experimental progress in synthesizing SA catalysts aside, the atomic-scale transformation mechanism from metal nanoparticles (NPs) to metal SAs and the stabilization mechanism of SA catalysts at high temperature remain elusive. Through systematic molecular dynamics simulations, for the first time, we reveal the atomic-scale mechanisms associated with the transformation of a metal NP into an array of stable SAs on a defective carbon surface at a high temperature, using Au as a model material. Simulations reveal the pivotal role of defects in the carbon surface in trapping and stabilizing the Au-SAs at high temperatures, which well explain previous experimental observations. Furthermore, reactive simulations demonstrate that the thermally stable Au-SAs exhibit much better catalyst activity than Au-NPs for the methane oxidation at high temperatures, in which the substantially reduced energy barriers for oxidation reaction steps are the key. Findings in this study offer mechanistic and quantitative guidance for material selection and optimal synthesis conditions to stabilize metal SA catalysts at high temperatures.npj Computational Materials (2020) 6:23 ; https://doi.

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Reversible and cooperative photoactivation of single-atom Cu/TiO2 photocatalysts

Cited by 529 publications

References 46 publications

Single‐Atom Iron Catalysts on Overhang‐Eave Carbon Cages for High‐Performance Oxygen Reduction Reaction

Single‐Atom Iron Catalysts on Overhang‐Eave Carbon Cages for High‐Performance Oxygen Reduction Reaction

Supported Noble‐Metal Single Atoms for Heterogeneous Catalysis

Stabilizing mechanism of single-atom catalysts on a defective carbon surface

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