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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Design of Single-Atom Co–N₅ Catalytic Site: A Robust Electrocatalyst for CO₂ Reduction with Nearly 100% CO Selectivity and Remarkable Stability

Journal of the American Chemical Society, Journal Year: 2018, Volume and Issue: 140(12), P. 4218 - 4221

Published: March 8, 2018

We develop an N-coordination strategy to design a robust CO2 reduction reaction (CO2RR) electrocatalyst with atomically dispersed Co-N5 site anchored on polymer-derived hollow N-doped porous carbon spheres. Our catalyst exhibits high selectivity for CO2RR CO Faradaic efficiency (FECO) above 90% over wide potential range from -0.57 -0.88 V (the FECO exceeded 99% at -0.73 and -0.79 V). The current density remained nearly unchanged after electrolyzing 10 h, revealing remarkable stability. Experiments functional theory calculations demonstrate single-atom is the dominating active center simultaneously activation, rapid formation of key intermediate COOH* as well desorption CO.

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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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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Core–shell structured catalysts for thermocatalytic, photocatalytic, and electrocatalytic conversion of CO₂

Chemical Society Reviews, Journal Year: 2020, Volume and Issue: 49(10), P. 2937 - 3004

Published: Jan. 1, 2020

Catalytic conversion of CO2 to produce fuels and chemicals is attractive in prospect because it provides an alternative fossil feedstocks the benefit converting cycling greenhouse gas on a large scale. In today's technology, converted into hydrocarbon Fischer-Tropsch synthesis via water shift reaction, but processes for direct such as methane, methanol, C2+ hydrocarbons or syngas are still far from large-scale applications processing challenges that may be best addressed by discovery improved catalysts-those with enhanced activity, selectivity, stability. Core-shell structured catalysts relatively new class nanomaterials allow controlled integration functions complementary materials optimised compositions morphologies. For conversion, core-shell can provide distinctive advantages addressing catalyst sintering activity loss reforming processes, insufficient product selectivity thermocatalytic hydrogenation, low efficiency photocatalytic electrocatalytic hydrogenation. preceding decade, substantial progress has been made synthesis, characterization, evaluation potential applications. Nonetheless, remain inexpensive, robust, regenerable this class. This review in-depth assessment these thermocatalytic, photocatalytic, valuable hydrocarbons.

Language: Английский

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Promoting electrocatalytic CO2 reduction to formate via sulfur-boosting water activation on indium surfaces

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

Published: Feb. 21, 2019

Electrocatalytic reduction of CO2 to fuels and chemicals is one the most attractive routes for utilization. Current catalysts suffer from low faradaic efficiency a CO2-reduction product at high current density (or reaction rate). Here, we report that sulfur-doped indium catalyst exhibits formate (>85%) in broad range (25-100 mA cm-2) electrocatalytic aqueous media. The formation rate reaches 1449 μmol h-1 cm-2 with 93% efficiency, highest value reported date. Our studies suggest sulfur accelerates by unique mechanism. Sulfur enhances activation water, forming hydrogen species can readily react produce formate. promoting effect chalcogen modifiers be extended other metal catalysts. This work offers simple useful strategy designing both active selective electrocatalysts reduction.

Language: Английский

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Cu-based nanocatalysts for electrochemical reduction of CO2

Nano Today, Journal Year: 2018, Volume and Issue: 21, P. 41 - 54

Published: May 21, 2018

Language: Английский

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Noble-Metal Based Random Alloy and Intermetallic Nanocrystals: Syntheses and Applications

Chemical Reviews, Journal Year: 2020, Volume and Issue: 121(2), P. 736 - 795

Published: Sept. 9, 2020

Precise control over the size, shape, composition, structure, and crystal phase of random alloy intermetallic nanocrystals has been intensively explored in technologically important applications recent years. Different from monometallic other types structural such as core-shell heterostructured nanocrystals, well-defined multimetallic exhibit unique intriguing physicochemical properties, serving ideal models for benefiting structure-to-property studies. As such, have attracted extensive attention interest scientific research shown huge potential various fields. In this review, we focus specifically on summarizing synthetic principles strategies developed to form with enhanced performance. Some representative examples are purposely selected emphasizing basic concepts mechanistic understanding. We then highlight fascinating properties widespread electrocatalysis, heterogeneous catalysis, optical photocatalysis, well magnetism conclude review by addressing prospects current challenges controlled synthesis nanocrystals.

Language: Английский

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Alloy Nanocatalysts for the Electrochemical Oxygen Reduction (ORR) and the Direct Electrochemical Carbon Dioxide Reduction Reaction (CO₂RR)

Advanced Materials, Journal Year: 2018, Volume and Issue: 31(31)

Published: Dec. 20, 2018

In the face of global energy challenge and progressing climate change, renewable systems components, such as fuel cells electrolyzers, which close energetic oxygen carbon cycles, have become a technology development priority. The electrochemical reduction reaction (ORR) direct dioxide (CO2RR) are important electrocatalytic processes that proceed at gas diffusion electrodes hydrogen CO2 respectively. However, their low catalytic activity (voltage efficiency), limited long-term stability, moderate product selectivity (related to Faradaic efficiency) remained challenges. To address these, suitable catalysts required. This review addresses current state research on Pt-based Cu-based nanoalloy electrocatalysts for ORR CO2RR, respectively, critically compares contrasts key performance parameters activity, selectivity, durability. particular, Pt nanoparticles alloyed with transition metals, post-transition metals lanthanides, discussed, well material characterization ORR. Then, bimetallic Cu reviewed organized according main generated by second metal. concludes perspective proposes future directions.

Language: Английский

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Electrochemical Energy Conversion on Intermetallic Compounds: A Review

ACS Catalysis, Journal Year: 2019, Volume and Issue: 9(3), P. 2018 - 2062

Published: Jan. 15, 2019

Structurally ordered intermetallic compounds possess unique chemical and physical properties, making them an interesting class of materials for application in electrocatalytic reactions. This Review comprises the work on used energy relevant electrocatalysis is structured by reactions scope, which are hydrogen evolution reaction (HER), electrochemical carbondioxide reduction (eCO2RR), oxygen (ORR), oxidation (HOR) as well formic acid (FAOR), methanol (MOR), ethanol (EtOR). Optimization pathways electrocatalysts, based adjustability materials, highlighted, experimental data provided a comparative manner, to provide overview, foundation, reference further development.

Language: Английский

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