Heterogeneous single-atom catalysis

Nature Reviews Chemistry, Journal Year: 2018, Volume and Issue: 2(6), P. 65 - 81

Published: May 24, 2018

Language: Английский

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Well-Defined Materials for Heterogeneous Catalysis: From Nanoparticles to Isolated Single-Atom Sites

Chemical Reviews, Journal Year: 2019, Volume and Issue: 120(2), P. 623 - 682

Published: Dec. 23, 2019

The use of well-defined materials in heterogeneous catalysis will open up numerous new opportunities for the development advanced catalysts to address global challenges energy and environment. This review surveys roles nanoparticles isolated single atom sites catalytic reactions. In second section, effects size, shape, metal-support interactions are discussed nanostructured catalysts. Case studies summarized illustrate dynamics structure evolution under certain reaction conditions. third we syntheses applications atomic anchored on different types supports. final part, conclude by highlighting catalyst gaining a fundamental understanding their active sites.

Language: Английский

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Low-Temperature CO₂ Methanation over CeO₂-Supported Ru Single Atoms, Nanoclusters, and Nanoparticles Competitively Tuned by Strong Metal–Support Interactions and H-Spillover Effect

ACS Catalysis, Journal Year: 2018, Volume and Issue: 8(7), P. 6203 - 6215

Published: May 24, 2018

CO2 hydrogenation for the acquisition of value-added chemicals is an economical means to deal with CO2-relevant environmental problems, among which reduction CH4 excellent model reaction investigating initial steps hydrogenation. For supported catalysts commonly used in such reactions, tailoring interfacial effect between metal centers and supporting materials so as obtain superior low-temperature methanation performance a significant but challenging subject. In this work, we altered size regimes Ru deposits Ru/CeO2 assemblies uncovered competitive relationship strong metal–support interactions (SMSI) H-spillover determining activities by some ex situ spectroscopic techniques coupled density functional theory (DFT) calculations. CeO2 nanowire single atoms, nanoclusters (ca. 1.2 nm size), large nanoparticles 4.0 show most outstanding activity 98–100% selectivity, turnover frequency (TOF) 7.41 × 10–3 s–1 at 190 °C. The negative order decreases their absolute values from atoms turns positive nanoparticles, while H2 follows reverse tendency. DRIFTS measurements demonstrate that dominant pathway CO route, carbonyls are critical intermediates active sites those Ce3+–OH near interfaces charge dissociation carbonyl hydrogenation, respectively. Meanwhile, strongest SMSI respectively encountered activation dehydration support surfaces suppressed correspondingly. two factors reach balance CeO2-supported nanoclusters, therefore maximized. A mechanistic understanding tuning would shed light on ingenious design utilize appropriate degree avoid possible suppressions take place extreme cases.

Language: Английский

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Identification of single-atom active sites in carbon-based cobalt catalysts during electrocatalytic hydrogen evolution

Nature Catalysis, Journal Year: 2018, Volume and Issue: 2(2), P. 134 - 141

Published: Dec. 13, 2018

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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Cascade anchoring strategy for general mass production of high-loading single-atomic metal-nitrogen catalysts

Nature Communications, Journal Year: 2019, Volume and Issue: 10(1)

Published: March 20, 2019

Abstract Although single-atomically dispersed metal-N x on carbon support (M-NC) has great potential in heterogeneous catalysis, the scalable synthesis of such single-atom catalysts (SACs) with high-loading is greatly challenging since loading and single-atomic dispersion have to be balanced at high temperature for forming . Herein, we develop a general cascade anchoring strategy mass production series M-NC SACs metal up 12.1 wt%. Systematic investigation reveals that chelation ions, physical isolation chelate complex upon loading, binding N-species elevated are essential achieving SACs. As demonstration, Fe-NC SAC shows superior electrocatalytic performance O 2 reduction Ni-NC exhibits activity CO reduction. The paves universal way produce stable high-density sites diverse high-performance applications.

Language: Английский

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

Nature Materials, Journal Year: 2019, Volume and Issue: 18(6), P. 620 - 626

Published: April 22, 2019

Language: Английский

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MXene (Ti₃C₂) Vacancy-Confined Single-Atom Catalyst for Efficient Functionalization of CO₂

Journal of the American Chemical Society, Journal Year: 2019, Volume and Issue: 141(9), P. 4086 - 4093

Published: Jan. 30, 2019

A central topic in single-atom catalysis is building strong interactions between single atoms and the support for stabilization. Herein we report preparation of stabilized catalysts via a simultaneous self-reduction stabilization process at room temperature using ultrathin two-dimensional Ti3–xC2TyMXene nanosheets characterized by abundant Ti-deficit vacancy defects high reducing capability. The therein form metal–carbon bonds with Ti3–xC2Ty are therefore onto sites previously occupied Ti. Pt-based catalyst (SAC) Pt1/Ti3–xC2Ty offers green route to utilizing greenhouse gas CO2, formylation amines, as C1 source organic synthesis. DFT calculations reveal that, compared Pt nanoparticles, on feature partial positive charges atomic dispersion, which helps significantly decrease adsorption energy activation silane, aniline, thereby boosting catalytic performance. We believe that these results would open up new opportunities fabrication SACs applications MXenes

Language: Английский

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Chemical reactivity under nanoconfinement

Nature Nanotechnology, Journal Year: 2020, Volume and Issue: 15(4), P. 256 - 271

Published: April 1, 2020

Language: Английский

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Atomic‐Level Modulation of Electronic Density at Cobalt Single‐Atom Sites Derived from Metal–Organic Frameworks: Enhanced Oxygen Reduction Performance

Angewandte Chemie International Edition, Journal Year: 2020, Volume and Issue: 60(6), P. 3212 - 3221

Published: Oct. 30, 2020

Demonstrated here is the correlation between atomic configuration induced electronic density of single-atom Co active sites and oxygen reduction reaction (ORR) performance by combining density-functional theory (DFT) calculations electrochemical analysis. Guided DFT calculations, a MOF-derived catalyst with optimal Co1 -N3 PS moiety incorporated in hollow carbon polyhedron (Co1 PS/HC) was designed synthesized. PS/HC exhibits outstanding alkaline ORR activity half-wave potential 0.920 V superior kinetics record-level kinetic current an ultralow Tafel slope 31 mV dec-1 , exceeding that Pt/C almost all non-precious electrocatalysts. In acidic media still surpasses Pt/C. This work offers atomic-level insight into relationship site catalytic properties, promoting rational design efficient catalysts.

Language: Английский

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