Metal Catalysts for Heterogeneous Catalysis: From Single Atoms to Nanoclusters and Nanoparticles

Chemical Reviews, Journal Year: 2018, Volume and Issue: 118(10), P. 4981 - 5079

Published: April 16, 2018

Metal species with different size (single atoms, nanoclusters, and nanoparticles) show catalytic behavior for various heterogeneous reactions. It has been shown in the literature that many factors including particle size, shape, chemical composition, metal–support interaction, metal–reactant/solvent interaction can have significant influences on properties of metal catalysts. The recent developments well-controlled synthesis methodologies advanced characterization tools allow one to correlate relationships at molecular level. In this Review, electronic geometric structures single nanoparticles will be discussed. Furthermore, we summarize applications types reactions, CO oxidation, selective hydrogenation, organic electrocatalytic, photocatalytic We compare results obtained from systems try give a picture how work reactions perspectives future directions toward better understanding entities unifying manner.

Language: Английский

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Progress and Perspectives of Electrochemical CO₂ Reduction on Copper in Aqueous Electrolyte

Chemical Reviews, Journal Year: 2019, Volume and Issue: 119(12), P. 7610 - 7672

Published: May 22, 2019

To date, copper is the only heterogeneous catalyst that has shown a propensity to produce valuable hydrocarbons and alcohols, such as ethylene ethanol, from electrochemical CO2 reduction (CO2R). There are variety of factors impact CO2R activity selectivity, including surface structure, morphology, composition, choice electrolyte ions pH, cell design. Many these often intertwined, which can complicate discovery design efforts. Here we take broad historical view different aspects their complex interplay in catalysis on Cu, with purpose providing new insights, critical evaluations, guidance field regard research directions best practices. First, describe various experimental probes complementary theoretical methods have been used discern mechanisms by products formed, next present our current understanding reaction networks for Cu. We then analyze two key attempts alter selectivity Cu: nanostructuring formation bimetallic electrodes. Finally, offer some perspectives future outlook CO2R.

Language: Английский

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Single-Atom Catalysts: Synthetic Strategies and Electrochemical Applications

Joule, Journal Year: 2018, Volume and Issue: 2(7), P. 1242 - 1264

Published: July 1, 2018

Language: Английский

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Cocatalysts for Selective Photoreduction of CO₂into Solar Fuels

Chemical Reviews, Journal Year: 2019, Volume and Issue: 119(6), P. 3962 - 4179

Published: Feb. 14, 2019

Photoreduction of CO2 into sustainable and green solar fuels is generally believed to be an appealing solution simultaneously overcome both environmental problems energy crisis. The low selectivity challenging multi-electron photoreduction reactions makes it one the holy grails in heterogeneous photocatalysis. This Review highlights important roles cocatalysts selective photocatalytic reduction using semiconductor catalysts. A special emphasis this review placed on key role, design considerations modification strategies for photoreduction. Various cocatalysts, such as biomimetic, metal-based, metal-free, multifunctional ones, their are summarized discussed, along with recent advances area. provides useful information highly photo(electro)reduction electroreduction complements existing reviews various photocatalysts.

Language: Английский

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Design of N-Coordinated Dual-Metal Sites: A Stable and Active Pt-Free Catalyst for Acidic Oxygen Reduction Reaction

Journal of the American Chemical Society, Journal Year: 2017, Volume and Issue: 139(48), P. 17281 - 17284

Published: Nov. 14, 2017

We develop a host-guest strategy to construct an electrocatalyst with Fe-Co dual sites embedded on N-doped porous carbon and demonstrate its activity for oxygen reduction reaction in acidic electrolyte. Our catalyst exhibits superior performance, comparable onset potential (Eonset, 1.06 vs 1.03 V) half-wave (E1/2, 0.863 0.858 than commercial Pt/C. The fuel cell test reveals (Fe,Co)/N-C outperforms most reported Pt-free catalysts H2/O2 H2/air. In addition, this cathode metal is stable long-term operation 50 000 cycles electrode measurement 100 h H2/air single operation. Density functional theory calculations reveal the favored activation of O-O, crucial four-electron reduction.

Language: Английский

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Single‐Atom Electrocatalysts

Angewandte Chemie International Edition, Journal Year: 2017, Volume and Issue: 56(45), P. 13944 - 13960

Published: May 24, 2017

Abstract Recent years have witnessed a dramatic increase in the production of sustainable and renewable energy. However, electrochemical performances various systems are limited, there is an intensive search for highly efficient electrocatalysts by more rational control over size, shape, composition, structure. Of particular interest studies on single‐atom catalysts (SACs), which sparked new interests electrocatalysis because their high catalytic activity, stability, selectivity, 100 % atom utilization. In this Review, we introduce innovative syntheses characterization techniques SACs, with focus applications oxygen reduction/evolution reaction, hydrogen evolution hydrocarbon conversion reactions fuel cells (electrooxidation methanol, ethanol, formic acid). The electrocatalytic performance further considered at atomic level underlying mechanisms discussed. ultimate goal tailoring single atoms applications.

Language: Английский

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Highly selective plasma-activated copper catalysts for carbon dioxide reduction to ethylene

Nature Communications, Journal Year: 2016, Volume and Issue: 7(1)

Published: June 30, 2016

Abstract There is an urgent need to develop technologies that use renewable energy convert waste products such as carbon dioxide into hydrocarbon fuels. Carbon can be electrochemically reduced hydrocarbons over copper catalysts, although higher efficiency required. We have developed oxidized catalysts displaying lower overpotentials for electroreduction and record selectivity towards ethylene (60%) through facile tunable plasma treatments. Herein we provide insight the improved performance of these by combining electrochemical measurements with microscopic spectroscopic characterization techniques. Operando X-ray absorption spectroscopy cross-sectional scanning transmission electron microscopy show oxides are surprisingly resistant reduction + species remain on surface during reaction. Our results demonstrate roughness oxide-derived plays only a partial role in determining catalytic performance, while presence key lowering onset potential enhancing selectivity.

Language: Английский

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Understanding activity and selectivity of metal-nitrogen-doped carbon catalysts for electrochemical reduction of CO2

Nature Communications, Journal Year: 2017, Volume and Issue: 8(1)

Published: Oct. 10, 2017

Direct electrochemical reduction of CO2 to fuels and chemicals using renewable electricity has attracted significant attention partly due the fundamental challenges related reactivity selectivity, its importance for industrial CO2-consuming gas diffusion cathodes. Here, we present advances in understanding trends CO electrocatalysis metal- nitrogen-doped porous carbons containing catalytically active M-N x moieties (M = Mn, Fe, Co, Ni, Cu). We investigate their intrinsic catalytic reactivity, turnover frequencies, faradaic efficiencies demonstrate that Fe-N-C especially Ni-N-C catalysts rival Au- Ag-based catalysts. model density functional theory correlate theoretical binding energies with experiments give reactivity-selectivity descriptors. This gives an atomic-scale mechanistic potential-dependent hydrocarbon selectivity from it provides predictive guidelines rational design selective carbon-based catalysts.Inexpensive electrocatalysts hold promise sustainable fuel production. authors report N-coordinated, non-noble metal-doped as efficient conversion.

Language: Английский

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Functional carbon nitride materials — design strategies for electrochemical devices

Nature Reviews Materials, Journal Year: 2017, Volume and Issue: 2(6)

Published: May 31, 2017

Language: Английский

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Strain-controlled electrocatalysis on multimetallic nanomaterials

Nature Reviews Materials, Journal Year: 2017, Volume and Issue: 2(11)

Published: Sept. 26, 2017

Language: Английский

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