Multiscale CO₂ Electrocatalysis to C₂₊ Products: Reaction Mechanisms, Catalyst Design, and Device Fabrication

Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(17), P. 10530 - 10583

Published: Aug. 17, 2023

Electrosynthesis of value-added chemicals, directly from CO2, could foster achievement carbon neutral through an alternative electrical approach to the energy-intensive thermochemical industry for utilization. Progress in this area, based on electrogeneration multicarbon products CO2 electroreduction, however, lags far behind that C1 products. Reaction routes are complicated and kinetics slow with scale up high levels required commercialization, posing significant problems. In review, we identify summarize state-of-art progress synthesis a multiscale perspective discuss current hurdles be resolved generation reduction including atomistic mechanisms, nanoscale electrocatalysts, microscale electrodes, macroscale electrolyzers guidelines future research. The review ends cross-scale links discrepancies between different approaches extensions performance stability issues arise industrial environment.

Language: Английский

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Rational design strategies of Cu-based electrocatalysts for CO2 electroreduction to C2 products

Journal of Energy Chemistry, Journal Year: 2022, Volume and Issue: 71, P. 63 - 82

Published: April 1, 2022

Language: Английский

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Oxyanion Engineering Suppressed Iron Segregation in Nickel–Iron Catalysts Toward Stable Water Oxidation

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(21)

Published: March 7, 2023

Nickel-iron catalysts represent an appealing platform for electrocatalytic oxygen evolution reaction (OER) in alkaline media because of their high adjustability components and activity. However, long-term stabilities under current density still remain unsatisfactory due to undesirable Fe segregation. Herein, a nitrate ion (NO3- ) tailored strategy is developed mitigate segregation, thereby improve the OER stability nickel-iron catalyst. X-ray absorption spectroscopy combined with theoretical calculations indicate that introducing Ni3 (NO3 )2 (OH)4 stable NO3- lattice conducive constructing interface FeOOH/Ni3 via strong interaction between incorporated . Time flight secondary mass spectrometry wavelet transformation analysis demonstrate catalyst greatly alleviates exhibiting considerably enhanced six-fold improvement over FeOOH/Ni(OH)2 without modification. This work represents momentous step toward regulating segregation stabilizing catalytic performances catalysts.

Language: Английский

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Local reaction environment in electrocatalysis

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(4), P. 2022 - 2055

Published: Jan. 1, 2024

Beyond conventional electrocatalyst engineering, recent studies have unveiled the effectiveness of manipulating local reaction environment in enhancing performance electrocatalytic reactions. The general principles and strategies environmental engineering for different processes been extensively investigated. This review provides a critical appraisal advancements aiming to comprehensively assess this emerging field. It presents interactions among surface structure, ions distribution electric field relation environment. Useful protocols such as interfacial reactant concentration, mass transport rate, adsorption/desorption behaviors, binding energy are in-depth discussed toward modifying Meanwhile, electrode physical structures cell configurations viable optimization methods environments. In combination with

Language: Английский

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Converting CO₂ into Value‐Added Products by Cu₂O‐Based Catalysts: From Photocatalysis, Electrocatalysis to Photoelectrocatalysis

Small, Journal Year: 2023, Volume and Issue: 19(19)

Published: Feb. 11, 2023

Abstract Converting CO 2 into value‐added products by photocatalysis, electrocatalysis, and photoelectrocatalysis is a promising method to alleviate the global environmental problems energy crisis. Among semiconductor materials applied in catalytic reduction, Cu O has advantages of abundant reserves, low price friendliness. Moreover, unique adsorption activation properties for , which conducive generation C 2+ through CC coupling. This review introduces basic principles reduction summarizes pathways 1 products. The factors affecting performance are further discussed from perspective reaction environment, medium, novel reactor design. Then, O‐based catalysts summarized several optimization strategies enhance their stability redox capacity discussed. Subsequently, application photocatalytic, electrocatalytic, photoelectrocatalytic described. Finally, opportunities, challenges research directions field presented, guidance its wide fields provided.

Language: Английский

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Strong Hydrogen-Bonded Interfacial Water Inhibiting Hydrogen Evolution Kinetics to Promote Electrochemical CO₂ Reduction to C₂₊

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(5), P. 3457 - 3465

Published: Feb. 19, 2024

Interfacial water is an important participant in electrochemical CO2 reduction (CO2RR), directly affecting the kinetics of hydrogenation steps occurring CO2RR and competitive hydrogen evolution reaction (HER). However, its structural composition dynamic are difficult to investigate due bulk interference bias dependence. Herein, we adopt situ vibration spectroscopy combined with molecular dynamics simulations probe change interfacial structure on electrified hydrophobic electrode surface further explore mechanism origin suppressed HER activity enhanced multicarbon products' selectivity. We reveal that near exhibits rigid intermolecular bonding interaction, degree which increases a potential. The strong bond makes it hard for reorientation leading longer metal–H distance, inhibits dissociation decreases *H coverage. Moderate coverage not only but also ensures intermediates realizing promoted C–C dimerization. A faradaic efficiency 75.2% products was ultimately achieved. Our results provide insights into understanding role controlling selectivity CO2RR.

Language: Английский

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Efficient Photothermal Anti‐/Deicing Enabled by 3D Cu_2‐xS Encapsulated Phase Change Materials Mixed Superhydrophobic Coatings

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(3)

Published: Nov. 23, 2023

Abstract Photothermal superhydrophobic surfaces are one of the most promising anti‐/deicing materials, yet they limited by low energy density and intermittent nature solar energy. Here, a coupling solution based on microencapsulated phase change materials (MPCMs) that integrates photothermal effect thermal storage is proposed. Dual‐shell octahedral MPCMs with Cu 2 O as first layer 3D 2‐x S second for time designed. By morphology manipulation shell, local surface plasmonic heating modulation realized, MPCM reveals full‐spectrum high absorption conversion efficiency up to 96.1%. The temperature enthalpy remain in good consistency after 200 cycles. Multifunctional phase‐change composite coatings fabricated combining hydrolyzed polycondensation products octadecyl trichlorosilane dual‐shell MPCM. multifunctional exhibit excellent performance under humidity conditions. This work not only provides new approach design high‐performance but also opens an avenue anti‐icing application coatings.

Language: Английский

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Tuning C1/C2 Selectivity of CO2 Electrochemical Reduction over in‐Situ Evolved CuO/SnO2 Heterostructure

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(40)

Published: July 24, 2023

Abstract Heterostructured oxides with versatile active sites, as a class of efficient catalysts for CO 2 electrochemical reduction (CO ER), are prone to undergo structure reconstruction under working conditions, thus bringing challenges understanding the reaction mechanism and rationally designing catalysts. Herein, we first time elucidate structural CuO/SnO potentials reveal intrinsic relationship between ER product selectivity in situ evolved heterostructures. At −0.85 V RHE , evolves Cu O/SnO high HCOOH (Faradaic efficiency 54.81 %). Mostly interestingly, it is reconstructed Cu/SnO 2‐x at −1.05 significantly improved Faradaic ethanol 39.8 %. In Raman spectra density functional theory (DFT) calculations that synergetic absorption *COOH *CHOCO intermediates interface favors formation *CO decreases energy barrier C−C coupling, leading ethanol.

Language: Английский

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Electronic Structure Design of Transition Metal-Based Catalysts for Electrochemical Carbon Dioxide Reduction

ACS Nano, Journal Year: 2024, Volume and Issue: 18(14), P. 9823 - 9851

Published: March 28, 2024

With the increasingly serious greenhouse effect, electrochemical carbon dioxide reduction reaction (CO2RR) has garnered widespread attention as it is capable of leveraging renewable energy to convert CO2 into value-added chemicals and fuels. However, performance CO2RR can hardly meet expectations because diverse intermediates complicated processes, necessitating exploitation highly efficient catalysts. In recent years, with advanced characterization technologies theoretical simulations, exploration catalytic mechanisms gradually deepened electronic structure catalysts their interactions intermediates, which serve a bridge facilitate deeper comprehension structure-performance relationships. Transition metal-based (TMCs), extensively applied in CO2RR, demonstrate substantial potential for further modulation, given abundance d electrons. Herein, we discuss representative feasible strategies modulate catalysts, including doping, vacancy, alloying, heterostructure, strain, phase engineering. These approaches profoundly alter inherent properties TMCs interaction thereby greatly affecting rate pathway CO2RR. It believed that rational design modulation fundamentally provide viable directions development toward conversion many other small molecules.

Language: Английский

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Photocatalysis toward Microplastics Conversion: A Critical Review

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(11), P. 8694 - 8719

Published: May 20, 2024

Microplastics (MPs, particle size < 5 mm) have become increasingly ubiquitous on Earth due to the cleavage and degradation of heavy use plastics. MPs recently been reported be detected in human blood, alveoli, breast milk, embryos, other organs, raising concerns about their environmental risks. Photocatalysis has identified as a potential means for conversion, which utilizes solar energy stimulate semiconductor photocatalyst. However, study photocatalytic conversion is still incubation period. This review overviews current state-of-the-art technologies conversion. Then, fundamental principles, challenges, analytical techniques, evaluation indexes reforming are highlighted. We systematically summarized recent advances key factors influencing performance. Finally, we propose some perspectives developing efficient systems MPs. will provide guideline applying technology MPs, significantly contribute this emerging research field.

Language: Английский

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