Single-Atom Catalysts across the Periodic Table

Chemical Reviews, Journal Year: 2020, Volume and Issue: 120(21), P. 11703 - 11809

Published: Oct. 21, 2020

Isolated atoms featuring unique reactivity are at the heart of enzymatic and homogeneous catalysts. In contrast, although concept has long existed, single-atom heterogeneous catalysts (SACs) have only recently gained prominence. Host materials similar functions to ligands in catalysts, determining stability, local environment, electronic properties isolated thus providing a platform for tailoring targeted applications. Within just decade, we witnessed many examples SACs both disrupting diverse fields catalysis with their distinctive substantially enriching our understanding molecular processes on surfaces. To date, term SAC mostly refers late transition metal-based systems, but numerous exist which other elements play key catalytic roles. This review provides compositional encyclopedia SACs, celebrating 10th anniversary introduction this term. By defining broadest sense, explore full elemental diversity, joining different areas across whole periodic table, discussing historical milestones recent developments. particular, examine coordination structures associated accessed through distinct single-atom–host combinations relate them main applications thermo-, electro-, photocatalysis, revealing trends element-specific evolution, host design, uses. Finally, highlight frontiers field, including multimetallic atom proximity control, possible multistep cascade reactions, identifying challenges, propose directions future development flourishing field.

Language: Английский

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Single-Atom Catalysts Based on the Metal–Oxide Interaction

Chemical Reviews, Journal Year: 2020, Volume and Issue: 120(21), P. 11986 - 12043

Published: Oct. 28, 2020

Metal atoms dispersed on the oxide supports constitute a large category of single-atom catalysts. In this review, supported catalysts are discussed about their synthetic procedures, characterizations, and reaction mechanism in thermocatalysis, such as water-gas shift reaction, selective oxidation/hydrogenation, coupling reactions. Some typical materials, including ferric oxide, cerium titanium dioxide, aluminum so on, intentionally mentioned for unique roles anchoring metal taking part catalytic The interactions between summarized to give picture how stabilize atomic centers, rationally tune geometric structures electronic states single atoms. Furthermore, several directions fabricating with improved performance proposed basis state-of-the-art understanding metal-oxide interactions.

Language: Английский

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Interface dynamics of Pd–CeO2 single-atom catalysts during CO oxidation

Nature Catalysis, Journal Year: 2021, Volume and Issue: 4(6), P. 469 - 478

Published: June 3, 2021

Language: Английский

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The Progress and Outlook of Metal Single-Atom-Site Catalysis

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(40), P. 18155 - 18174

Published: Sept. 29, 2022

Single-atom-site catalysts (SASCs) featuring maximized atom utilization and isolated active sites have progressed tremendously in recent years as a highly prosperous branch of catalysis research. Varieties SASCs been developed that show excellent performance many catalytic applications. The major goal SASC research is to establish feasible synthetic strategies for the preparation high-performance catalysts, achieve an in-depth understanding active-site structures mechanisms, develop practical with industrial value. This Perspective describes up-to-date development related such dual-atom-site (DASCs) nano-single-atom-site (NSASCs), analyzes current challenges encountered by these applications, proposes their possible future path.

Language: Английский

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Silver Single‐Atom Catalyst for Efficient Electrochemical CO₂ Reduction Synthesized from Thermal Transformation and Surface Reconstruction

Angewandte Chemie International Edition, Journal Year: 2020, Volume and Issue: 60(11), P. 6170 - 6176

Published: Dec. 4, 2020

Abstract We report an Ag 1 single‐atom catalyst (Ag /MnO 2 ), which was synthesized from thermal transformation of nanoparticles (NPs) and surface reconstruction MnO . The evolution process NPs to single atoms is firstly revealed by various techniques, including in situ ETEM, XRD DFT calculations. temperature‐induced the (211) (310) lattice plane critical firmly confine existing atoms; that is, treatment driving force for formation atoms. as‐obtained achieved 95.7 % Faradic efficiency at −0.85 V vs. RHE, coupled with long‐term stability electrochemical CO reduction reaction (CO RR). calculations indicated sites possessed high electronic density close Fermi Level could act exclusively as active RR. As a result, demonstrated remarkable performance RR, far surpassing conventional nanosized NP ) other reported Ag‐based catalysts.

Language: Английский

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Recent Advances in Catalytic Hydrosilylations: Developments beyond Traditional Platinum Catalysts

Angewandte Chemie International Edition, Journal Year: 2020, Volume and Issue: 60(2), P. 550 - 565

Published: July 15, 2020

Hydrosilylation reactions, which allow the addition of Si-H to C=C/C≡C bonds, are typically catalyzed by homogeneous noble metal catalysts (Pt, Rh, Ir, and Ru). Although excellent activity selectivity can be obtained, price, purification, residues these precious problems in silicone industry. Thus, a strong interest more sustainable for economic processes exists. In this respect, recently disclosed hydrosilylations using based on earth-abundant transition metals, example, Fe, Co, Ni, Mn, heterogeneous (supported nanoparticles single-atom sites) noteworthy. This minireview describes recent advances field.

Language: Английский

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Thermally Stable Single‐Atom Heterogeneous Catalysts

Advanced Materials, Journal Year: 2021, Volume and Issue: 33(50)

Published: March 25, 2021

Single-atom catalysts (SACs) have attracted extensive attention in fields related to energy, environment, and material sciences because of the high atom efficiency unique properties these materials. Many approaches hitherto been successfully established prepare SACs, including impregnation, pyrolysis-involved processes, trapping, coprecipitation. However, under typical reaction conditions, single atoms on tend migrate or agglomerate, forming nanoclusters nanoparticles, which lowers their surface free energy. Efforts are required develop strategies for improving thermal stability SACs while achieving excellent catalytic performance. In this Progress Report, recent advances development thermally durable single-atom heterogeneous discussed. Several important preparation stable described article. Fundamental understanding coordination structures prepared by methods is Furthermore, performances reviewed, activity stability. Finally, a perspective rapidly evolving research field provided.

Language: Английский

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Prospects of Heterogeneous Hydroformylation with Supported Single Atom Catalysts

Journal of the American Chemical Society, Journal Year: 2020, Volume and Issue: 142(11), P. 5087 - 5096

Published: March 6, 2020

The potential of oxide-supported rhodium single atom catalysts (SACs) for heterogeneous hydroformylation was investigated both theoretically and experimentally. Using high-level domain-based local-pair natural orbital coupled cluster singles doubles with perturbative triples contribution (DLPNO-CCSD(T)) calculations, stability catalytic activity were Rh atoms on different oxide surfaces. Atomically dispersed, supported synthesized MgO CeO2. While the CeO2-supported catalyst is found to be highly active, this not case MgO, most likely due increased confinement, as determined by extended X-ray absorption fine structure spectroscopy (EXAFS), that diminishes reactivity complexes MgO. This agrees well our computational investigation, where we find carbonyl hydride flat surfaces such CeO2(111) have activities comparable those molecular complexes. For a step edge MgO(301) surface, however, calculations show significantly reduced activity. At same time, predict stronger adsorption at higher coordinated site leads more stable catalyst. Keeping balance between appears main challenge catalysts. In addition chemical bonding complex support, confinement experienced active plays an important role

Language: Английский

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Advanced Support Materials and Interactions for Atomically Dispersed Noble‐Metal Catalysts: From Support Effects to Design Strategies

Advanced Energy Materials, Journal Year: 2021, Volume and Issue: 12(1)

Published: Nov. 21, 2021

Abstract Indisputably, noble‐metal single atom catalysts (SACs) are one of the most popular research topics in field catalysis because their low cost, ultrahigh atomic utilization, and distinctive performance for a wide variety catalytic reactions. Support materials play vital role preparation SACs. Thus, diverse support have been developed very rapidly elaborately designed last few years. In this review, effects SACs first systematically introduced, including anchoring effects, strong metal–support interactions, synergistic effects. Moreover, recent advances classified discussed detail with focus on mechanism. Importantly, design strategies advanced supports summarized guiding development utilization materials. To conclude possible future directions put forward to help overcome current issues facing

Language: Английский

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Design of Single-Atom Catalysts and Tracking Their Fate Using Operando and Advanced X-ray Spectroscopic Tools

Chemical Reviews, Journal Year: 2022, Volume and Issue: 123(1), P. 379 - 444

Published: Nov. 23, 2022

The potential of operando X-ray techniques for following the structure, fate, and active site single-atom catalysts (SACs) is highlighted with emphasis on a synergetic approach both topics. absorption spectroscopy (XAS) related have become fascinating tools to characterize solids they can be applied almost all transition metals deriving information about symmetry, oxidation state, local coordination, many more structural electronic properties. SACs, newly coined concept, recently gained much attention in field heterogeneous catalysis. In this way, one achieve minimum use metal, theoretically highest efficiency, design only site-so-called single catalysts. While sites are not easy especially under operating conditions, XAS as probe together complementary methods (infrared spectroscopy, electron microscopy) ideal research area prove structure these dynamic changes during reaction. review, starting from their fundamentals, various conventional photon in/out discussed detailed mechanistic situ/operando studies. We systematically summarize strategies SACs outline exploration supported by density functional theory (DFT) calculations recent machine learning tools.

Language: Английский

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