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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Transition Metal Complexes as Catalysts for the Electroconversion of CO₂: An Organometallic Perspective

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(21), P. 11628 - 11686

Published: Jan. 19, 2021

The electrocatalytic transformation of carbon dioxide has been a topic interest in the field CO2 utilization for long time. Recently, area seen increasing dynamics as an alternative strategy to catalytic hydrogenation reduction. While many studies focus on direct electron transfer molecule at electrode material, molecular transition metal complexes solution offer possibility act catalysts transfer. C1 compounds such monoxide, formate, and methanol are often targeted main products, but more elaborate transformations also possible within coordination sphere center. This perspective article will cover selected examples illustrate categorize currently favored mechanisms electrochemically induced promoted by homogeneous complexes. insights be corroborated with concepts elementary steps organometallic catalysis derive potential strategies broaden diversity products.

Language: Английский

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Optimizing the Electrocatalytic Selectivity of Carbon Dioxide Reduction Reaction by Regulating the Electronic Structure of Single‐Atom M‐N‐C Materials

Advanced Functional Materials, Journal Year: 2022, Volume and Issue: 32(19)

Published: Feb. 9, 2022

Abstract Electrochemical carbon dioxide reduction reaction (CO 2 RR) is an efficient strategy to relieve global environmental and energy issues by converting excess CO from the atmosphere value‐added products. Atomically dispersed metal‐nitrogen‐doped (M‐N‐C) materials are superior catalysts for electrocatalytic RR because of 100% atomic utilization, unsaturated coordination configuration, relatively uniform active sites, well‐defined adjustable structure centers. However, electrochemical a great challenge due process involving proton‐coupled multi‐electron transfer with high barrier, which leads unsatisfactory selectivity targeted product, especially C2 products (e.g., C H 4 5 OH). Here, authors systematically summarize effective means, including reasonable selection isolated metal regulation environment atoms, fabrication dimetallic single‐atom sites attaining optimal geometric electronic structures M‐N‐C further correlate these catalytic various C1 CH ) in RR. Moreover, constructive strategies optimize provided. Finally, challenges future research directions application proposed.

Language: Английский

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Harnessing the power of machine learning for carbon capture, utilisation, and storage (CCUS) – a state-of-the-art review

Energy & Environmental Science, Journal Year: 2021, Volume and Issue: 14(12), P. 6122 - 6157

Published: Jan. 1, 2021

A review of the state-of-the-art applications machine learning for CO 2 capture, transport, storage, and utilisation.

Language: Английский

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Enabling storage and utilization of low-carbon electricity: power to formic acid

Energy & Environmental Science, Journal Year: 2021, Volume and Issue: 14(3), P. 1194 - 1246

Published: Jan. 1, 2021

Power to formic acidviaCO₂hydrogenation or electrochemical CO₂reduction has great potential enable a complete cycle with acid power for the storage and utilization of low-carbon electricity at scale multi-gigatonnes per year.

Language: Английский

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2022 roadmap on low temperature electrochemical CO₂ reduction

Journal of Physics Energy, Journal Year: 2022, Volume and Issue: 4(4), P. 042003 - 042003

Published: June 13, 2022

Abstract Electrochemical CO 2 reduction (CO R) is an attractive option for storing renewable electricity and the sustainable production of valuable chemicals fuels. In this roadmap, we review recent progress in fundamental understanding, catalyst development, engineering scale-up. We discuss outstanding challenges towards commercialization electrochemical R technology: energy efficiencies, selectivities, low current densities, stability. highlight opportunities establishing rigorous standards benchmarking performance, advances operando characterization, discovery new materials high value products, investigation phenomena across multiple-length scales application data science doing so. hope that collective perspective sparks research activities ultimately bring us a step closer low- or zero-emission carbon cycle.

Language: Английский

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Ligand Engineering in Nickel Phthalocyanine to Boost the Electrocatalytic Reduction of CO₂

Advanced Functional Materials, Journal Year: 2021, Volume and Issue: 32(10)

Published: Dec. 1, 2021

Abstract Designing and synthesizing efficient molecular catalysts may unlock the great challenge of controlling CO 2 reduction reaction (CO RR) with precision. Nickel phthalocyanine (NiPc) appears as a promising candidate for this task due to its adjustable Ni active‐site. However, pristine NiPc suffers from poor activity stability RR owing adsorption activation at bare site. Here, ligand‐tuned strategy is developed enhance catalytic performance unveil ligand effect on RR. Theoretical calculations experimental results indicate that electron‐donating substituents (hydroxyl or amino) can induce electronic localization site which greatly enhances activation. Employing optimal catalyst—an amino‐substituted NiPc—to convert into in flow cell achieve an ultrahigh selectivity 99.8% current densities up −400 mA cm −2 . This work offers novel regulate structure active sites by design discloses ligand‐directed catalysis tailored highly

Language: Английский

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Robust Biological Hydrogen‐Bonded Organic Framework with Post‐Functionalized Rhenium(I) Sites for Efficient Heterogeneous Visible‐Light‐Driven CO₂ Reduction

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(16), P. 8983 - 8989

Published: Jan. 26, 2021

Abstract A robust 2,2′‐bipyridine (bpy)‐derived biological hydrogen‐bonded framework (HOF‐25) has been realized depending on guanine‐quadruplex with the assistance of π‐π interaction, which reacts Re(CO) 5 Cl to give a post‐functionalized HOF‐25‐Re. X‐ray absorption fine structure spectroscopic study HOF‐25‐Re confirms covalent attachment Re(bpy)(CO) 3 segments this HOF. Robust and recycled bearing photocatalytic centers displays good heterogeneous catalytic activity towards carbon dioxide photoreduction in presence [Ru(bpy) ]Cl 2 triisopropanolamine CH CN under visible‐light irradiation, both high CO production rate 1448 μmol g −1 h selectivity 93 %. Under same conditions, experimental turnover number (50) is about 8 times as that homogeneous control Cl. The sustainably regenerated via crystallization post‐modification processes shows recovered performance.

Language: Английский

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Crossing the Valley of Death: From Fundamental to Applied Research in Electrolysis

JACS Au, Journal Year: 2021, Volume and Issue: 1(5), P. 527 - 535

Published: April 12, 2021

The growing societal and political focus on the use of environmentally friendly technologies has led to an ever-increasing interest in electrolysis scientific communities. This development is reflected by plethora candidate catalysts for hydrogen oxygen evolution reactions, as well CO2 reduction reaction, reported literature. However, almost none them entered stage application yet. Likewise, reports process engineering inadequately address utilization these catalysts, electrode cell concepts, that might be suitable market. Evidently, a closer collaboration between chemists engineers from industry academia desirable speed up disruptive technologies. Herein, we elucidate critical parameters highlight necessary aspects accelerate industrially relevant capable fulfilling forthcoming challenges related energy conversion storage. aim this Perspective, composed industrial academic partners, critically question current undertakings encourage researchers strike interdisciplinary research pathways.

Language: Английский

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Photocatalytic Systems for CO₂ Reduction: Metal-Complex Photocatalysts and Their Hybrids with Photofunctional Solid Materials

Accounts of Chemical Research, Journal Year: 2022, Volume and Issue: 55(7), P. 978 - 990

Published: March 7, 2022

ConspectusPhotocatalytic CO2 reduction is a critical objective in the field of artificial photosynthesis because it can potentially make total solution for global warming and shortage energy carbon resources. We have successfully developed various highly efficient, stable, selective photocatalytic systems using transition metal complexes as both photosensitizers catalysts. The molecular architectures constructing efficient are discussed herein. As typical example, mixed system ring-shaped Re(I) trinuclear complex photosensitizer fac-[Re(bpy)(CO)3{OC2H4N(C2H4OH)2}] catalyst selectively photocatalyzed to CO with highest quantum yield 82% turnover number (TON) over 600. Not only rare noble metals but also earth abundant ones, such Mn(I), Cu(I), Fe(II) be used central cations. In case Cu(I) dinuclear fac-Mn(bpy)(CO)3Br catalyst, formation HCOOH from was 57% TONCO+HCOOH exceeded 1300.Efficient supramolecular photocatalysts reduction, which units connected through bridging ligand, were removing diffusion control on collisions between catalyst. Supramolecular photocatalysts, [Ru(N∧N)3]2+-type or Ru(II) each other an alkyl chain, efficiently solutions. Mechanistic studies time-resolved IR electrochemical measurements provided architecture photocatalysts. A Ru(II)-Re(I) photocatalyst constructed according this even when fixed solid materials. Harnessing property two types hybrid developed, namely, light-harvesting capabilities photoelectrochemical reduction.Introduction into should important intensity solar light shone earth's surface relatively low. Periodic mesoporous organosilica, methyl acridone groups embedded silica framework harvesters, combined phosphonic acid anchoring groups. hybrid, photons absorbed by approximately 40 transferred one unit, then, commenced.To use water electron donor, we combining metal-complex semiconductor that display high photooxidation powers, sequentially semiconductor, resulting oxidation power. Various dye-sensitized photocathodes comprising p-type electrodes developed. Full cells these n-type photoanodes achieved visible source reductant. Drastic improvement reported.The results presented Account clearly indicate construct very selective, durable supramolecular-photocatalyst useful especially owing rapid transfer On basis findings, photoactive These hybridizations add new functions systems, harvesting.

Language: Английский

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