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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Recent Advances in Carbon Dioxide Hydrogenation to Methanol via Heterogeneous Catalysis

Chemical Reviews, Journal Year: 2020, Volume and Issue: 120(15), P. 7984 - 8034

Published: Feb. 12, 2020

The utilization of fossil fuels has enabled an unprecedented era prosperity and advancement well-being for human society. However, the associated increase in anthropogenic carbon dioxide (CO2) emissions can negatively affect global temperatures ocean acidity. Moreover, are a limited resource their depletion will ultimately force one to seek alternative sources maintain sustainable economy. Converting CO2 into value-added chemicals fuels, using renewable energy, is promising approaches this regard. Major advances energy-efficient conversion potentially alleviate emissions, reduce dependence on nonrenewable resources, minimize environmental impacts from portions displaced. Methanol (CH3OH) important chemical feedstock be used as fuel internal combustion engines cells, well platform molecule production fuels. As approaches, thermocatalytic hydrogenation CH3OH via heterogeneous catalysis attracted great attention past decades. progress been made development various catalysts including metals, metal oxides, intermetallic compounds. In addition, efforts also put forth define catalyst structures nanoscale by taking advantage nanostructured materials, which enables tuning composition modulation surface endows more catalytic performance comparison bulk materials prepared traditional methods. Despite these achievements, significant challenges still exist developing robust with good long-term stability. review, we provide comprehensive overview recent area, especially focusing structure–activity relationship, importance combining measurements, situ characterization, theoretical studies understanding reaction mechanisms identifying key descriptors designing improved catalysts.

Language: Английский

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Atomically Precise Noble Metal Nanoclusters as Efficient Catalysts: A Bridge between Structure and Properties

Chemical Reviews, Journal Year: 2019, Volume and Issue: 120(2), P. 526 - 622

Published: March 22, 2019

Improving the knowledge of relationship between structure and properties is fundamental in catalysis. Recently, researchers have developed a variety well-controlled methods to synthesize atomically precise metal nanoclusters (NCs). NCs shown high catalytic activity unique selectivity many reactions, which are related their ultrasmall size, abundant unsaturated active sites, electronic different from that traditional nanoparticles (NPs). More importantly, because definite monodispersity, they used as model catalysts reveal correlation catalyst performance at atomic scale. Therefore, this review aims summarize recent progress on catalysis provide potential theoretical guidance for rational design high-performance catalysts. First brief summary synthetic strategies characterization provided. Then primary focus review-the role catalysis-is illustrated experimental perspectives, particularly electrocatalysis, photocatalysis, photoelectric conversion, organic reactions. Finally, main challenges opportunities examined deep understanding key steps with goal expanding application range NCs.

Language: Английский

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Domino electroreduction of CO2 to methanol on a molecular catalyst

Nature, Journal Year: 2019, Volume and Issue: 575(7784), P. 639 - 642

Published: Nov. 27, 2019

Language: Английский

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Electrocatalysis for CO₂conversion: from fundamentals to value-added products

Chemical Society Reviews, Journal Year: 2021, Volume and Issue: 50(8), P. 4993 - 5061

Published: Jan. 1, 2021

This timely and comprehensive review mainly summarizes advances in heterogeneous electroreduction of CO₂: from fundamentals to value-added products.

Language: Английский

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Electro- and Solar-Driven Fuel Synthesis with First Row Transition Metal Complexes

Chemical Reviews, Journal Year: 2019, Volume and Issue: 119(4), P. 2752 - 2875

Published: Feb. 15, 2019

The synthesis of renewable fuels from abundant water or the greenhouse gas CO2 is a major step toward creating sustainable and scalable energy storage technologies. In last few decades, much attention has focused on development nonprecious metal-based catalysts and, in more recent years, their integration solid-state support materials devices that operate water. This review surveys literature 3d molecular focuses immobilization heterogeneous supports for electro-, photo-, photoelectrocatalytic aqueous media. first sections highlight benchmark homogeneous systems using proton reducing transition metal as well commonly employed methods catalyst immobilization, including discussion supporting anchoring groups. subsequent elaborate productive associations between wide range substrates based carbon, quantum dots, oxide surfaces, semiconductors. molecule–material hybrid are organized “dark” cathodes, colloidal photocatalysts, photocathodes, figures merit discussed alongside system stability integrity. final section extends scope this to prospects challenges targeting catalysis beyond “classical” H2 evolution reduction C1 products, by summarizing cases higher-value products N2 reduction, Cx>1 utilization, other reductive organic transformations.

Language: Английский

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Advanced Electrocatalysts with Single-Metal-Atom Active Sites

Chemical Reviews, Journal Year: 2020, Volume and Issue: 120(21), P. 12217 - 12314

Published: Nov. 2, 2020

Electrocatalysts with single metal atoms as active sites have received increasing attention owing to their high atomic utilization efficiency and exotic catalytic activity selectivity. This review aims provide a comprehensive summary on the recent development of such single-atom electrocatalysts (SAECs) for various energy-conversion reactions. The discussion starts an introduction different types SAECs, followed by overview synthetic methodologies control dispersion atomically resolved characterization using state-of-the-art microscopic spectroscopic techniques. In recognition extensive applications electrocatalytic studies are dissected in terms important electrochemical reactions, including hydrogen evolution reaction (HER), oxygen (OER), reduction (ORR), carbon dioxide (CO2RR), nitrogen (NRR). Examples SAECs deliberated each case performance, structure-property relationships, enhancement mechanisms. A perspective is provided at end section about remaining challenges opportunities targeted reaction.

Language: Английский

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Molecular electrocatalysts can mediate fast, selective CO ₂ reduction in a flow cell

Science, Journal Year: 2019, Volume and Issue: 365(6451), P. 367 - 369

Published: July 25, 2019

Practical electrochemical carbon dioxide (CO2) conversion requires a catalyst capable of mediating the efficient formation single product with high selectivity at current densities. Solid-state electrocatalysts achieve CO2 reduction reaction (CO2RR) densities ≥ 150 milliamperes per square centimeter (mA/cm2), but maintaining selectivities and efficiencies remains challenge. Molecular CO2RR catalysts can be designed to low overpotentials only irrelevant commercial operation. We show here that cobalt phthalocyanine, widely available molecular catalyst, mediate CO in zero-gap membrane flow reactor > 95% mA/cm2 The revelation work efficiently under these operating conditions illuminates distinct approach for optimizing electrolyzers.

Language: Английский

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Surface and Interface Control in Nanoparticle Catalysis

Chemical Reviews, Journal Year: 2019, Volume and Issue: 120(2), P. 1184 - 1249

Published: Oct. 3, 2019

The surface and interfaces of heterogeneous catalysts are essential to their performance as they often considered be active sites for catalytic reactions. With the development nanoscience, ability tune interface nanostructures has provided a versatile tool optimization catalyst. In this Review, we present control nanoparticle in context oxygen reduction reaction (ORR), electrochemical CO2 (CO2 RR), tandem catalysis three sections. first section, start with activity ORR on nanoscale then focus approaches optimize Pt-based catalyst including using alloying, core-shell structure, high area open structures. section RR, where composition plays dominant role, cover its fundamentals different nanosized metal catalysts. For catalysis, adjacent single nanostructure catalyze sequential reactions, describe concept principle, synthesis methodology, application

Language: Английский

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Scalable Production of Efficient Single-Atom Copper Decorated Carbon Membranes for CO₂ Electroreduction to Methanol

Journal of the American Chemical Society, Journal Year: 2019, Volume and Issue: 141(32), P. 12717 - 12723

Published: July 26, 2019

Electrocatalytic reduction reaction of CO2 (CO2RR) is an effective way to mitigate energy and environmental issues. However, very limited catalysts are capable converting resources into high-value products such as hydrocarbons or alcohols. Herein, we first propose a facile strategy for the large-scale synthesis isolated Cu decorated through-hole carbon nanofibers (CuSAs/TCNFs). This CuSAs/TCNFs membrane has excellent mechanical properties can be directly used cathode CO2RR, which could generate nearly pure methanol with 44% Faradaic efficiency in liquid phase. The self-supporting structure greatly reduces embedded metal atoms produces abundant efficient single atoms, actually participate eventually causing -93 mA cm-2 partial current density C1 more than 50 h stability aqueous solution. According DFT calculations, possess relatively higher binding *CO intermediate. Therefore, further reduced like methanol, instead being easily released from catalyst surface CO product. report may benefit design high-yield single-atom other electrocatalytic reactions.

Language: Английский

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